Publicaciones

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Efficient Nebulization and Pulmonary Biodistribution of Polymeric Nanocarriers in an Acute Lung Injury Preclinical Model

Digital.CSIC. Repositorio Institucional del CSIC
  • Solé Porta, Anna
  • Areny Balagueró, Aina
  • Camprubí Rimblas, Marta
  • Fernández Fernández, Elena
  • O’Sullivan, Andrew
  • Giannoccari, Rossella
  • MacLoughlin, Ronan
  • Closa, Daniel
  • Artigas, Antonio
  • Roig Serra, Anna
Acute respiratory distress syndrome (ARDS) is a clinical syndrome characterized by acute hypoxemic respiratory failure. Pneumonia and sepsis are the most common causes, turning ARDS into a critical public health problem. Despite recent advances in pharmacological strategies, clinical trials have not demonstrated a reduction in ARDS-associated mortality. This is in part connected to the singularity of the pulmonary physiological barrier, which hampers drug delivery, specifically at distal areas. To this aim, the use of polymeric nanocarriers as a platform for the efficient delivery of therapeutics to the lungs by nebulization is introduced. Herein, poly(lactic-co-glycolic acid) (PLGA) nanocapsules (NCs) loaded with human serum albumin, as an inhalable nanotherapeutic are prepared. The production of stable NCs aerosols in the inhalable range is achieved using a commercial device, while the nanocarrier's physicochemical parameters are only minimally altered after nebulization. Importantly, in vivo studies with healthy and acute lung injury animals show that after inhalation, the NCs are homogeneously distributed throughout the lungs, arriving at the distal areas. The NCs are internalized by alveolar type II cells, avoiding macrophage-mediated lung clearance. These features make the PLGA NCs excellent vehicles for noninvasive pulmonary delivery, facilitating a ready-to-be-used nanomedicine., Figures were created using Biorender.com. Grants PID2021-122645OB-I00 and CEX2023001263-S (“Severo Ochoa” Program for Center of Excellence in R&D) funded by MCIN/AEI/10.13039/501100011033 and by FEDER, “A way of making Europe”, as well as the Generalitat de Catalunya (2021SGR00446 project) are kindly acknowledged. Also, this study is supported by the Fundación Ramón Areces (CIVP19S8207), I3PT (CIR2020/028), and CIBERES. A.S.-P. acknowledges the Ph.D. scholarship (FPU21/04142) in the framework of the Materials Science Ph.D. program of the UAB., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Electronic Transport Modulation in Ultrastrained Silicon Nanowire Devices

Digital.CSIC. Repositorio Institucional del CSIC
  • Bartmann, Maximilian G.
  • Glassner, Sebastian
  • Sistani, Masiar
  • Rurali, Riccardo
  • Palummo, Maurizia
  • Cartoixà, Xavier
  • Smoliner, Jürgen
  • Lugstein, Alois
In this work, we explore the effect of ultrahigh tensile strain on electrical transport properties of silicon. By integrating vapor-liquid-solid-grown nanowires into a micromechanical straining device, we demonstrate uniaxial tensile strain levels up to 9.5%. Thereby the triply degenerated phonon dispersion relation at the Γ-point of silicon disentangle and the longitudinal phonon modes are used to precisely determine the extent of mechanical strain. Simultaneous electrical transport measurements showed a significant enhancement in the electrical conductance. Aside from considerable reduction of the Si bulk resistivity due to strain-induced band gap narrowing, comparison with quasi-particle GW calculations further reveals that the effective Schottky barrier height at the electrical contacts undergoes a substantial reduction. For these reasons, nanowire devices with ultrastrained channels may be promising candidates for future applications of high-performance silicon-based devices., The authors gratefully acknowledge financial support by the Austrian Science Fund (FWF): Project No. P29729-N27. R.R. acknowledges financial support from MCIN/AEI/10.13039/501100011033 under grant PID2020–119777GB-I00, the Severo Ochoa Centres of Excellence Program under grant CEX2023-001263-S, and the Generalitat de Catalunya under grant 2021 SGR01519. M.P. acknowledges Union─NextGenerationEU under the Italian National Center 1 on HPC–Spoke 6: “Multiscale Modelling and Engineering Applications”. X.C acknowledges financial support by Spain’s Ministerio de Ciencia e Innovación under grant no. PID2021-127840NB-I00 (MICINN/AEI/FEDER, UE)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Multifunctional self-refrigerated multivariate {GdLn} (Ln = Dy, Tb, Tb/Eu) metal-organic frameworks

Digital.CSIC. Repositorio Institucional del CSIC
  • Li, Zhen
  • Arauzo, Ana
  • Roscini, Claudio
  • Giner Planas, José
  • Bartolomé, Elena
Multivariate metal-organic frameworks (MOFs) containing multiple lanthanide ions present a compelling avenue for developing versatile materials with tailored properties. In this work, we synthesized “self-refrigerated” multifunctional carborane-based MOFs of formula unit {[(GdLn)3(mCB-L)4(NO3)(DMF)x]n·Solv} strategically combining Gd3+ ions, known for their ability to achieve large magnetocaloric effects (MCE), with various lanthanides (Ln = Dy, Tb, Eu, Tb/Eu) intended to act as Single Molecule Magnet (SMM) or/and luminescent units. The intricate magnetic, thermal, and optical properties of these multivariate Ln-MOFs were unraveled through a comprehensive characterization employing dc and ac magnetometry, X-ray Absorption Spectroscopy (XAS), X-ray Magnetic Circular Dichroism (XMCD), and luminescence measurements. Element-selective XAS-XMCD technique proved instrumental in elucidating the magnetic properties of the individual lanthanides, and their contribution to the macroscopic properties of the MOFs. We demonstrate that Gd1.5Ln1.5 (Ln = Tb, Dy) MOFs exhibit multifunctionality, incorporating MCE, field-induced magnetic relaxation dominated by the anisotropic ion, and green emission for Ln = Tb. Conversely, Gd1.5Ln1.5 (Ln = Eu, Eu/Tb) MOFs display MCE, field-induced SMM behavior associated with Gd, and red/yellow luminescent emission for Ln = Eu and Eu/Tb substitutions, respectively. Our findings significantly contribute to our understanding of “complex magnetic molecular materials” and set a pathway for the design of multifunctional multi-lanthanide MOFs endowed with tailored properties for various technological applications., This work was financially supported by MINECO (PID2022-138492NB-I00 and PID2022-136892NB-I00), the Generalitat de Catalunya (2021/SGR/00442), and the Gobierno de Aragón (RASMIA E12-23). EB and JGP acknowledges financial support from the State Investigation Agency, through the Severo Ochoa Programme for Centres of Excellence in R&D (CEX2023-001263-S). Zhen Li acknowledges the China Scholarship Council (CSC) for his PhD grant (201808310071). Authors would like to acknowledge the use of Servicio General de Apoyo a la Investigación-SAI, Universidad de Zaragoza. XAS and XMCD experiments were performed at the BOREAS beamline of the ALBA synchrotron with the support of ALBA staff (experiment number 2022085925)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Unravelling the origin of thermal anisotropy in PdSe2

Digital.CSIC. Repositorio Institucional del CSIC
  • Xu, Kai
  • Martínez Armesto, Luis
  • Svetlik, Josef
  • Sierra, Juan F.
  • Marinova, Vera
  • Dimitrov, Dimitre
  • Graczykowski, Bartlomiej
  • Rurali, Riccardo
  • Valenzuela, Sergio O.
  • Reparaz, J. Sebastian
We acknowledge financial support from the Spanish Ministerio de Ciencia e Innovación (MICINN) for its support through Grant CEX2023-001263-S and CEX2021-001214-S in the framework of the Spanish Severo Ochoa Centre of Excellence program, and Grants PID2020-119777GB-I00 (THERM2MAIN), and PDC2021-121814-I00 (COVEQ). We also acknowledge Grant 2021-SGR-004 4 4 (NANOPTO) from the Catalan agency AGAUR. This research was also partially supported by MICIU/AEI/10.13039/501100 011033 through R&D projects PID2022-143162OB-I00 funded by and ERDF/EU, PCI2019-103739 and Co-Funded by the European Union. K X acknowledges a fellowship (CSC201806950006) from China Scholarship Council and the PhD program in Materials Science from Universitat Autònoma de Barcelona in which he was enrolled. J S acknowledges funding from the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie Grant Agreement No. 754558. J F S acknowledges support from MINECO under Contract RYC2019-028368-I/AEI/10.13039/50110 001103. B G acknowledges financial support National Center for Research and Development Grant No. EIG CONCERT-JAPAN/9/91/PETITE/2023. V M and D D acknowledge the funding from the Bulgarian Science Fund under Project Numbers FNI КП-06-ДO 02/2 and FNI КП-06-ДO 02/3, within the framework of the M-ERA program Project 'Functional 2D materials and heterostructures for hybrid spintronic-memristive devices'., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




In situ shaping of intricated 3D bacterial cellulose constructs using sacrificial agarose and diverted oxygen inflow

Digital.CSIC. Repositorio Institucional del CSIC
  • Abol-Fotouh, Deyaa
  • Al-Hagar, Ola E.A.
  • Roig Serra, Anna
Bacterial cellulose (BC) is gathering increased attention due to its remarkable physico-chemical features. The high biocompatibility, hydrophilicity, and mechanical and thermal stability endorse BC as a suitable candidate for biomedical applications. Nonetheless, exploiting BC for tissue regeneration demands three-dimensional, intricately shaped implants, a highly ambitious endeavor. This challenge is addressed here by growing BC within a sacrificial viscoelastic medium consisting of an agarose gel cast inside polydimethylsiloxane (PDMS) molds imprinted with the features of the desired implant. BC produced with and without agarose has been compared through SEM, TGA, FTIR, and XRD, probing the mild impact of the agarose on the BC properties. As a first proof of concept, a PDMS mold shaped as a doll's ear was used to produce a BC perfect replica, even for the smallest features. The second trial comprised a doll face imprinted on a PDMS mold. In that case, the BC production included consecutive deactivation and activation of the aerial oxygen stream. The resulting BC face clone fitted perfectly and conformally with the template doll face, while its rheological properties were comparable to those of collagen. This streamlining concept conveys to the biosynthesized nanocelluloses broader opportunities for more advanced prosthetics and soft tissue engineering uses., DAF is grateful to his beloved spouse Eman Kassab for her unlimited and inspirational support, and for The Egyptian Ministry of Higher Education and Scientific Research for funding postdoctoral scholarship. OEA is grateful to the Egyptian Atomic Energy Authority (EAEA) for supporting this work. AR acknowledges the project PID2021-122645OB-I00 funded by MCIN/AEI/10.13039/501100011033 by “ERDF A way of making Europe” and the “Severo Ochoa” Programme for the Center of Excellence in R&D (
CEX2023001263-S
), and the Generalitat de Catalunya (
2021SGR00446
grant)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Impacts of graphene quantum dots on the optical, electrical and thermal properties of the archetypal conducting polymer PEDOT:PSS

Digital.CSIC. Repositorio Institucional del CSIC
  • Kong, Minghua
  • Garriga Bacardi, Miquel
  • Reparaz, J. Sebastian
  • Alonso Carmona, M. Isabel
We investigated the optical properties and thermal conductivity of blade-coated graphene quantum dots (GQDs)/PEDOT:PSS hybrid thin films by varying the content of GQDs. The optical properties were determined by spectroscopic ellipsometry in the range of 1.2–5.5 eV. Two dispersion models were used to analyze the optical properties of the films: the Bruggeman effective medium approximation (BEMA) for the hybrid films, and the Drude model combined with a Lorentzian oscillator for both the pure and the hybrid films, which provides insight into their electrical properties. As a novel finding, we observed that the optical anisotropy of PEDOT:PSS (Aldrich 483095) films is reduced after incorporating GQDs. Moreover, dedoping of the PEDOT chains is demonstrated upon increasing the content of GQDs within the hybrid films. Furthermore, the thermal conductivity shows a two-fold decrease as the GQDs fraction increases from 0 to 10 wt%. This result is understood considering that the GQDs act as local scattering centers, resulting in a decrease of the thermal conductivity., The authors acknowledge funding from the Spanish Ministerio de Ciencia e Innovación (MICINN) through grants
PDC2021-121475-I00
and
PID2020-119777GB-I00
and the Spanish Severo Ochoa Centre of Excellence program
CEX2019-000917-S and CEX2023-001263-S
, as well as AGAUR, Generalitat de Catalunya, Spain, grant
2021-SGR-00444
. M.K. is grateful to the UAB PhD program in Materials Science in which she was enrolled and the China Scholarship Council for funding (
CSC 201809370071
). M.K. is sincerely thankful to Bernhard Dörling and Denise Estrada-Wiese for their corrections to the English and helpful comments. We thank Agustín Mihi and Mariano Campoy-Quiles for their constant support and ideas. We acknowledge the assistance of the ICMAB-CSIC Scientific & Technical Services: Nanoquim Platform, Scanning Probe Microscopy, Electron Microscopy, and X-ray Diffraction., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Charge density waves and electron-hole instabilities of the hidden-nesting materials P4⁢W12⁢O44, 𝛾- and 𝜂−Mo4⁢O11

Digital.CSIC. Repositorio Institucional del CSIC
  • Guster, Bogdan
  • Pruneda, Miguel
  • Ordejón, Pablo
  • Canadell, Enric
  • Pouget, Jean-Paul
The origin of the charge density wave (CDW) instabilities in the isostructural but not isoelectronic octahedral layers of the three-dimensional solids 𝛾−Mo4⁢O11 and P4⁢W12⁢O44 is discussed on the basis of first-principles density functional theory calculations. These layers contain three different and superposed one-dimensional (1D) systems (two diagonal and one horizontal) associated with the three 𝑡2⁢𝑔 orbitals of the transition metal in octahedral coordination. Because of the special topology of the layers the three 1D systems are practically independent (hidden nesting) and the Lindhard function contains three different lines of intensity maxima associated with each of them. Clear cusps (six for P4⁢W12⁢O44 and four for 𝛾−Mo4⁢O11) occur at the intersections of these intensity lines. The wave vector of the structural modulations associated with some of these cusps from our calculations is in good agreement with the observed CDW wave vectors. The nature of the different modulations is analyzed on the basis of the calculated thermal dependence of intrachain and interchain coherence lengths of the diffuse lines associated with the diagonal and horizontal chains. Modulation in the diagonal chains is found to be more favorable than in the horizontal chain. The same type of wave vector is selected for 𝛾−Mo4⁢O11 and P4⁢W12⁢O44 despite having a different band filling. The coupling of the electronic instability to the phonon spectra and the relationship between the nature of the high-temperature modulation with the width of the octahedral layers is discussed. Among the two Magnéli phases the interlayer coupling is found to be somewhat stronger in 𝜂−Mo4⁢O11. The relationship with other hidden-nesting series of materials as the rare-earth tellurides is commented., This paper owes much to numerous structural studies on 2D oxides and bronzes by P. Foury-Leylekian (Orsay) to whom we are very indebted. The authors also thank A. Minelli (Oak Ridge) for useful discussions concerning her IXS studies on the MPTB𝑝 and E. Duverger-Nédellec (Bordeaux) for sharing the results of her structural studies. B.G. acknowledges computational resources provided by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds de la Recherche Scientifique (F.R.S.-FNRS) under Grant No. 2.5020.11 and the Tier-1 Lucia supercomputer of the Walloon Region, infrastructure funded by the Walloon Region under the Grant Agreement No. 1910247. B.G., M.P., and P.O. acknowledge support from Grant No. PID2022-139776NB-C62 funded by the Spanish MCIN/AEI/10.13039/501100011033 and by the ERDF, a way of making Europe and the Severo Ochoa program from Spanish MINECO (Grant No. CEX2021-001214-S). E.C. was supported by Grant No. PID2022-139776NB-C61 funded by the Spanish MCIN/AEI/10.13039/501100011033 and AEI through the Severo Ochoa MaTrans42 (Grant No. CEX2023-0001263-S) Excellence Centre distinction. B.G., M.P., P.O., and E.C. acknowledge support from Generalitat de Catalunya (CERCA program and Grant No. 2021SGR01519)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Imaging the adsorption sites of organic molecules on metallic surfaces by an adaptive tunnelling current feedback

Digital.CSIC. Repositorio Institucional del CSIC
  • Martín Jiménez, Daniel
  • Zhong, Qigang
  • Schirmeisen, André
  • Ebeling, Daniel
Atomic force microscopy (AFM) allows submolecular resolution imaging of organic molecules deposited on a surface by using CO-functionalized qPlus sensors under ultrahigh vacuum and low temperature conditions. However, the experimental determination of the adsorption sites of these organic molecules requires the precise identification of the atomic structure of the surface on which they are adsorbed. Here, we develop an automation method for AFM imaging that provides in a single image both, submolecular resolution on organic molecules and atomic resolution on the surrounding metallic surface. The method is based on an adaptive tunnelling current feedback system that is regulated according to the response of the AFM observables, which guarantees that both the molecules and the surface atoms are imaged under optimum conditions. Therewith, the approach is suitable for imaging adsorption sites of several adjacent and highly mobile molecules such as 2-iodotriphenylene on Ag(111) in a single scan. The proposed method with the adaptive feedback system facilitates statistical analysis of molecular adsorption geometries and could in the future contribute to autonomous AFM imaging as it adapts the feedback parameters depending on the sample properties., We thank Dr Sebastian Ahles and Prof. Hermann A Wegner (Institute of Organic Chemistry, Justus Liebig University Giessen) for synthesizing and providing the ITP molecules. This research was funded by Deutsche Forschungsgemeinschaft (DFG) via Grants EB 535/1-1, EB 535/2-1, EB 535/4-1, SCHI 619/13, SCH 619/14-1 and the European Regional Development Fund via grant FPG991 (Innovation Labs for High-performance Materials). Martin-Jimenez acknowledges funding from the European Union Next Generation EU together with the 'Plan de Recuperación, Transformación y Resiliencia' from the Spanish Government and La Generalitat de Catalunya via 'Programa de Fondos Complementarios de Materiales Avanzados' PRTR-C17.I1 (InCAEM). All authors also gratefully acknowledge financial support the LOEWE Program of Excellence of the Federal State of Hesse (LOEWE Focus Group PriOSS 'Principles of On-Surface Synthesis')., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Evaluation of power cycling and charge capacity in Cu/Zn batteries with unwired bipolar electrodes immersed

Digital.CSIC. Repositorio Institucional del CSIC
  • Mosqueda, Marc
  • Bengoa, Leandro Nicolás
  • Goñi, Sandro M.
  • Casañ Pastor, Nieves
-Data to be open with Origin Pro
-Data obtained from experiments above as described in paper
-Cu and Zn electrodes in Copper and zinc suphate electrolyte as described in the paper, subject to charge discharge cycles, Evaluation of changes in cahrage caapcity, power, current densities in Cu/Zn in neutral pH, in presence of bipolar unwired electrodes in various configurations, Capacities, current densities, CV , impedances and power measurements, Peer reviewed




Dimensional crossover of microscopic magnetic metasurfaces for magnetic field amplification

Digital.CSIC. Repositorio Institucional del CSIC
  • Lejeune, Nicolas
  • Fourneau, Emile
  • Barrera, Aleix
  • Morris, O.
  • Leonard, Oscar
  • Arregi, Jon Ander
  • Navau, Carles
  • Uhlíř, Vojtěch
  • Bending, Simon John
  • Palau, Anna
  • Silhanek, Alejandro
Transformation optics applied to low frequency magnetic systems have been recently implemented to design magnetic field concentrators and cloaks with superior performance. Although this achievement has been amply demonstrated theoretically and experimentally in bulk 3D macrostructures, the performance of these devices at low dimensions remains an open question. In this work, we numerically investigate the non-monotonic evolution of the gain of a magnetic metamaterial field concentrator as the axial dimension is progressively shrunk. In particular, we show that in planar structures, the role played by the diamagnetic components becomes negligible, whereas the paramagnetic elements increase their magnetic field channeling efficiency. This is further demonstrated experimentally by tracking the gain of superconductor-ferromagnet concentrators through the superconducting transition. Interestingly, for thicknesses where the diamagnetic petals play an important role in the concentration gain, they also help to reduce the stray field of the concentrator, thus limiting the perturbation of the external field (invisibility). Our findings establish a roadmap and set clear geometrical limits for designing low dimensional magnetic field concentrators., This work was supported by the Fonds de la Recherche Scientifique - FNRS under the program Grant Nos. PDR T.0204.21 and CDR J.0176.22, EraNet-CHISTERA Grant No. R.8003.21, the Spanish Ministry of Science and Innovation MCIN/AEI/10.13039/501100011033/through CHIST-ERA Grant Nos. PCI2021-122028-2A and PCI2021-122083-2A cofinanced by the European Union Next Generation EU/PRTR, HTSUPERFUN Grant No. PID2021-124680OB-I00 cofinanced by ERDF as a way of making Europe, MAGNETOLIGHT TED2021-130402B-IOO, “Severo Ochoa” Programme CEX2023-001263-S and PID2019-104670GB-I00 of the Agencia Estatal de Investigación/Fondo Europeo de Desarrollo Regional (UE), and by COST (European Cooperation in Science and Technology) [www.cost.eu] through COST Action Grant No. SUPERQUMAP (CA 21144). Access to the CEITEC Nano Research Infrastructure was supported by the Ministry of Education, Youth, and Sports (MEYS) of the Czech Republic under Project No. Czech NanoLab (LM2023051). J.A.A. and V.U. acknowledge the support from the TACR EraNet CHIST-ERA Project No. MetaMagIC TH77010001. S. J. B. was supported by the Engineering and Physical Sciences Research Council (EPSRC) in the United Kingdom under Grant No. EP/W022680/1. N. L. acknowledges the support from FRS-FNRS (Research Fellowships FRIA). The work of E. Fourneau has been financially supported by the FWO and F.R.S.-FNRS under the Excellence of Science (EOS) Project No. O.0028.22., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Moving microscopic objects with self-disassembly

Digital.CSIC. Repositorio Institucional del CSIC
  • Amabilino, David B.
News & Views section, Etching supramolecular fibres causes nanoscale motion of an attached bead from the etched end towards the middle of the fibre., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Electrostatic interaction between SARS-CoV-2 and charged surfaces: Spike protein evolution changed the game

Digital.CSIC. Repositorio Institucional del CSIC
  • Domingo, Marc
  • Guzmán, Horacio
  • Kanduc, Matej
  • Faraudo, Jordi
Previous works show a key role of electrostatics for the SARS-CoV-2 virus in aspects such as virus-cell interactions or virus inactivation by ionic surfactants. Electrostatic interactions depend strongly on the variant since the charge of the Spike protein (responsible for virus - environment interactions) evolved across the variants from the highly negative Wild Type (WT) to the highly positive Omicron variant. The distribution of the charge also evolved from diffuse to highly localized. These facts suggest that SARS-CoV-2 should interact strongly with charged surfaces in a way that changed during the virus evolution. This question is studied here by computing the electrostatic interaction between WT, Delta and Omicron Spike proteins with charged surfaces using a new method (based on Debye-Huckel theory) that provides efficiently general results as a function of the surface charge density σ. We found that the interaction of the WT and Delta variant spikes with charged surfaces is dominated by repulsive image forces proportional to σ2 originated at the protein/water interface. On the contrary, the Omicron variant shows a distinct behaviour, being strongly attracted to negatively charged surfaces and repelled from positively charged ones. Therefore, the SARS-CoV-2 virus has evolved from being repelled by charged surfaces to being efficiently adsorbing to negatively charged ones., This work was supported by Grant No. PID2021-124297NB-C33 funded by MICIU/AEI/
10.13039/501100011033, the “Severo Ochoa” Grant No. CEX2023-001263-S for Centers of
Excellence awarded to ICMAB, and the FPI under Grant No. PRE2020-093689 awarded to
M.D.We also thank the Government of Catalonia (AGAUR) under Grant No. 2021SGR01519.
H.V.G. acknowledges financial support from the Maria Zambrano Grant No. CA6/RSUE/2022-
00108 and Ramon y Cajal grant No. RYC2022-038082-I. M.K. acknowledges financial support
from the Slovenian Research and Innovation Agency ARIS (contracts P1-0055 and J1-4382).
We thank the CESGA supercomputing center for computer time and technical support at
the Finisterrae supercomputer. We thank Dr. Fiona L. Kearns (UCSD) for discussions
regarding the spike protein structures.
M.D. is enrolled in the Material Sciences Ph.D. program of the Universitat Aut`onoma de
Barcelona., No




Thermal Stability and Purity of Graphene and Carbon Nanotubes: Key Parameters for Their Thermogravimetric Analysis (TGA)

Digital.CSIC. Repositorio Institucional del CSIC
  • Martincic, Markus
  • Sandoval, Stefania
  • Oró, Judith
  • Tobias, Gerard
Thermal analysis is widely employed for the characterization of nanomaterials. It encompasses a variety of techniques that allow the evaluation of the physicochemical properties of a material by monitoring its response under controlled temperature. In the case of carbon nanomaterials, such as carbon nanotubes and graphene derivatives, thermogravimetric analysis (TGA) is particularly useful to determine the quality and stability of the sample, the presence of impurities and the degree of functionalization or doping after post-synthesis treatments. Furthermore, TGA is widely used to evaluate the thermal stability against oxidation by air, which can be, for instance, enhanced by the purification of the material and by nitrogen doping, finding application in areas where a retarded combustion of the material is required. Herein, we have evaluated key parameters that play a role in the data obtained from TGA, namely, gas flow rate, sample weight and temperature rate, used during the analysis. We found out that the heating rate played the major role in the process of combustion in the presence of air, inducing an increase in the temperature at which the oxidation of CNTs starts to occur, up to ca. 100 °C (from 1 °C min−1 to 50 °C min−1). The same trend was observed for all the evaluated systems, namely N-doped CNTs, graphene produced by mechanical exfoliation and N-doped reduced graphene samples. Other aspects, like the presence of impurities or structural defects in the evaluated samples, were analyzed by TGA, highlighting the versatility and usefulness of the technique to provide information of structural aspects and properties of carbon materials. Finally, a set of TGA parameters are recommended for the analysis of carbon nanomaterials to obtain reliable data., This work was supported by State Investigation Agency, through PID2020-113805 GB-I00 and the Severo Ochoa Programme for Centres of Excellence in R&D (CEX2023-001263-S). S.S. acknowledges funding from the postdoctoral fellowship programme Beatriu de Pinós, funded by the Secretary of Universities and Research (Government of Catalonia) and Horizon 2020 programme of research and innovation of the European Union under the Marie Sklodowska-Curie grant agreement Nº 801370., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Electromigration-driven weak resistance switching in high-temperature superconducting devices

Digital.CSIC. Repositorio Institucional del CSIC
  • Marinković, Stefan
  • Stoffels, Daniel
  • Collienne, Simon
  • Fernández Rodríguez, Alejandro
  • Mestres, Narcís
  • Palau, Anna
  • Silhanek, Alejandro V.
Complex oxides are at the heart of modern functional material developments. In particular, the perovskite 𝐴⁢𝐵⁢O3 structure is seen in compounds used in oxide solar cells, resistive memories, fuel cell catalysts, superconducting tapes, quantum bits, and programmable magnets, making it one of the most studied material families. One important advantage of these systems is that their properties may be controlled in situ to change between various electronic states, usually by means of thermal or electric conditioning. In this work, we investigate the two-terminal resistive switching properties of the perovskitelike oxide YBa2⁢Cu3⁢O7−𝛿 when the system is driven by electric current. We perform all-electrical switching to characterize and control low-amplitude resistance changes, and we implement finite-element modeling to explain how these effects can be properly accounted for by oxygen-vacancy counterflow induced by electric bias. The presented research sheds light on the bulk displacement of oxygen atoms in perovskite materials with potential for sensing and memory technologies., The authors acknowledge support from Fonds de la
Recherche Scientifique - FRS-FNRS (Research Fellowship
ASP), the European COST action SUPERQUMAP (CA
21144), and the Spanish Ministry of Science and Innovation
MCIN/AEI/10.13039/501100011033/ through the “Severo
Ochoa” Programme for Centres of Excellence MaTrans42
CEX2023-001263-S, HTSUPERFUN PID2021-124680OBI00 funded by ERDF, “A way of making Europe.” The Spanish
Nanolito networking project (RED2022-134096-T) and Catalan government (2021-SGR-00440) are also acknowledged.
S.M. acknowledges support from FRS-FNRS Research Fellowship ASP under Grant No. 1.A.320.21F., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Circularly Polarized Photoluminescence characteristics of emiters placed on a nanophotonic platform

Digital.CSIC. Repositorio Institucional del CSIC
  • Mendoza Carreño, José
  • Mihi, Agustín
"Circular dichroism
The differential transmittance measurements were carried out in a custom-made optical setup. A white-light tungsten halogen lamp (Ocean Optics, HL-2000-HP, FL, USA) is coupled to a silver reflective collimator (RC08SMA-P01, Thorlabs) and used as an excitation light source. The light beam is passed through a Glan-Thompson Calcite Polarizer (GTH10M, Thorlabs) and directed to a super achromatic quarter wave-plate (SAQWP05M-700, Thorlabs) oriented at ±π/4 compared to the polarization direction on a rotation mount (ELL14, Thorlabs) to obtain a circularly polarized light beam. The optical elements are automatically controlled by custom software (LabView NXG). The sample is positioned at the focal plane of a pair of 4x objectives (RMS4X, NA = 0.1, Olympus). Finally, the transmitted light is fiber-coupled to a spectrometer (Ocean Optics, QEPro-FL).

Steady-state circularly polarized photoluminescence
Chiral photoluminescence is characterized using the same optical elements as for the dichroic transmittance but reversed in order. First, the emitted chiral photoluminescence is directed to a quarter wave-plate (10RP52-1B, Newport) oriented at ±π/4 and then to a linear polarizer (20LP-VIS-B, Newport), filtering one of the circular components. The excitation source consisted of a 200ps pulsed laser source (LDH-P-C-405 laser driven with a PDL 800B driver with 5–80 MHz repetition rate)) with its wavelength peak at 405nm.
In the case of the unpolarized excitation study, the light source used for excitation was an unpolarized LED centered at 405nm (M405L4, Thorlabs) coupled to a 4x (RMS4X, NA=0.1, Olympus) objective used to collimate the diverging emitted beam and refocused with an achromatic 50mm lens upon the metasurface.


Time-resolved circularly polarized photoluminescence
The optical set-up used for the time-resolved photoluminescence was PicoQuant Time
Correlated Single Photon Counting system (Time Harp 260 PICO board, 25 ps temporal resolution; PMA Hybrid 40 detector, 250 ps response time; 405 nm LDH-P-C-405 laser driven with a PDL 800B driver with 5–80 MHz repetition rate) equipped with a compact monochromator (Solar Laser Systems). Photoluminescence lifetimes were retrieved using the PicoQuant FluoFit Pro software, and fitting the PL decay data accounting for instrument response function.", Peer reviewed




Seeing ferroelectric phase transitions

Digital.CSIC. Repositorio Institucional del CSIC
  • Fina, Ignasi
  • Sánchez Barrera, Florencio
Real-time atomic-scale imaging reveals the presence of reversible transitions between ferroelectric and non-ferroelectric phases during electric stimuli, enabling the possibility for reliability improvement in ferroelectric materials compatible with complementary metal–oxide–semiconductors., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




A high-performance electromagnetic code to simulate high-temperature superconductors

Digital.CSIC. Repositorio Institucional del CSIC
  • Soba, Alejandro
  • Fernández Serracanta, Oriol
  • Lorenzo, José
  • Garcin, Diego
  • Houzeaux, Guillaume
  • Lamas, Neil
  • Granados, Xavier
  • Mantsinen, Mervi M.
Superconductivity is a physical phenomenon of some materials that allow them to conduct electrical current without resistance. This property has a wide range of applications. In particular, type-II high-temperature superconductors appear promising for building strong electromagnets carrying large amounts of current in the extreme conditions foreseen for future fusion reactors. However, their fabrication and related experiments are highly expensive and complex. Therefore, there is an increasing need for numerical models to guide the design optimization of superconducting cables and to predict their performance. In this work, we present a new code to simulate high-temperature superconductors (HTS) based on the edge finite element discretization of Maxwell's equations in the time domain using the widely adopted H-formulation in the superconductor analysis community. This code is integrated in the High-Performance Computing (HPC) Alya suite and obtain an excellent performance up to 1024 processors in MareNostrum 4 supercomputer. This capacity allows to us to solve a wide variate of problems in big domains in relatively reduce amount of computer time, being a promising tool to aboard HTS coils design problems. Furthermore, validations against experimental data are presented and code results for superconducting tapes with different magnetic properties are analyzed., This work is part of the FusionCAT project (001-P-001722) which has been 50% co-financed by the European Fund for Regional Development of the European Union within the framework of the 2014–2020 ERDF Operational Program of Catalonia, with the support of the Generalitat of Catalonia. In addition, it has been partly co-financed by grant PID2019-110854RB-I00 funded by MCIN/AEI/10.13039/501100011033 ., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Compelling DNA intercalation through 'anion-anion' anti-coulombic interactions: boron cluster self-vehicles as promising anticancer agents

Digital.CSIC. Repositorio Institucional del CSIC
  • Gutiérrez Gálvez, Laura
  • García Mendiola, Tania
  • Lorenzo, Encarnación
  • Nuez Martinez, Miquel
  • Ocal, Carmen
  • Yan, Shunya
  • Teixidor, Francesc
  • Pinheiro, Teresa
  • Marques, Fernanda
  • Viñas, Clara
Anticancer drugs inhibit DNA replication by intercalating between DNA base pairs, forming covalent bonds with nucleotide bases, or binding to the DNA groove. To develop safer drugs, novel molecular structures with alternative binding mechanisms are essential. Stable boron hydrides offer a promising alternative for cancer therapy, opening up additional options like boron neutron capture therapy based on 10B and thermal neutron beams or proton boron fusion therapy using 11B and proton beams. These therapies are more efficient when the boron compound is ideally located inside cancer cells, particularly in the nucleus. Current cancer treatments often utilize small, polycyclic, aromatic, planar molecules that intercalate between ds-DNA base pairs, requiring only a spacing of approximately 0.34 nm. In this paper, we demonstrate another type of intercalation. Notably, [3,3'-Fe(1,2-C2B9H11)2]-, ([o-FESAN]-), a compact 3D molecule measuring 1.1 nm × 0.6 nm, can as well intercalate by strong non-bonding interactions preferentially with guanine. Unlike known intercalators, which are positive or neutral, [o-FESAN]- is a negative species and when an [o-FESAN]- molecule approaches the negatively charged DNA phosphate chain an anion-anion interaction consistently anti-electrostatic via Ccluster-H⋯O-P bonds occurs. Then, when more molecules approach, an elongated outstandingly self-assembled structure of [o-FESAN]--[o-FESAN]- forms moving anions towards the interthread region to interact with base pairs and form aggregates of four [o-FESAN]- anions per base pair. These aggregates, in this environment, are generated by Ccluster-H⋯O-C, N-H⋯H-B and Ccluster-H⋯H-B interactions. The ferrabis(dicarbollide) boron-rich small molecules not only effectively penetrate the nucleus but also intercalate with ds-DNA, making them promising for cancer treatment. This amphiphilic anionic molecule, used as a carrier-free drug, can enhance radiotherapy in a multimodal perspective, providing healthcare professionals with improved tools for cancer treatment. This work demonstrates these findings with a plethora of techniques., Authors received support from the Spanish Ministerio de Economía y Competitividad (PID2020-116728RB-I00, PID2022-136802NB-I00, RED2022-134120-T and TED2021-129738B-I00), the Generalitat de Catalunya (2017SGR1720). L. Gutiérrez-Gálvez was supported by FPU19/06309 grant from the Spanish Ministry of Universities. S. Y. was supported by the China Scholarship Council (CSC) under Grant No. 202006990034., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Giant spin-charge conversion in ultrathin films of the MnPtSb half-Heusler compound

Digital.CSIC. Repositorio Institucional del CSIC
  • Longo, Emanuele
  • Markou, Anastasios
  • Felser, Claudia
  • Belli, Matteo
  • Serafini, Andrea
  • Targa, Paolo
  • D. Codegoni
  • Fanciulli, Marco
  • Mantovan, Roberto
main text: 17 pages (with 4 figures), plus additional 8 pages of Supplementary Information, Half-metallic half-Heusler compounds with strong spin-orbit-coupling and
broken inversion symmetry in their crystal structure are promising materials
for generating and absorbing spin-currents, thus enabling the electric
manipulation of magnetization in energy-efficient spintronic devices. In this
work, we report the spin-to-charge conversion in sputtered ultrathin films of
the half-Heusler compound MnPtSb with thickness (t) in the range from 1 to 6
nm. A combination of X-ray and transmission electron microscopy measurements
evidence the epitaxial nature of these ultrathin non-centrosymmetric MnPtSb
films, with a clear (111)-orientation obtained on top of (0001) single-crystal
sapphire substrates. The study of the thickness (t)-dependent magnetization
dynamics of the MnPtSb(t)/Co(5nm)/Au(5nm) heterostructure revealed that the
MnPtSb compound can be used as an efficient spin current generator, even at
film thicknesses as low as 1 nm. By making use of spin pumping FMR, we measure
a remarkable t-dependent spin-charge conversion in the MnPtSb layers, which
clearly demonstrate the interfacial origin of the conversion. When interpreted
as arising from the inverse Edelstein effect (IEE), the spin-charge conversion
efficiency extracted at room temperature for the thinnest MnPtSb layer reaches
{\lambda}IEE~3 nm, representing an extremely high spin-charge conversion
efficiency at room temperature. The still never explored ultrathin regime of
the MnPtSb films studied in this work and the discover of their outstanding
functionality are two ingredients which demonstrate the potentiality of such
materials for future applications in spintronics., The authors thank Edouard Lesne for discussions. The authors acknowledge the Horizon 2020 project SKYTOP “Skyrmion-Topological Insulator and Weyl Semimetal Technology” (FETPROACT-2018-01, n. 824123). E.L., A.M., and R.M. conceived the experiment. E.L. conducted all the BFMR, SP-FMR, and XRD measurements. E.L. and M.B. developed the BFMR and SP-FMR set-up and performed the analysis of the FMR-based results. M.F. supervised the FMR activity at the University of Milano-Bicocca laboratory. A.M. produced the samples and performed magnetometry measurements. A.S., P.T., and D.C. performed and analyzed the TEM measurements. C.F. coordinated the samples growth activity at the Max Planck Institute. R.M. coordinated the research activity. E. L. wrote the manuscript. All authors discussed and reviewed the manuscript and the Supporting Information. [Correction added on June 28, 2024, after first online publication: Affiliations has been updated.], With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Unlocking potential diabetes therapeutics: Insights into alpha-glucosidase inhibition, Identification of promising Lysosomal α-Glucosidase (rhGAA) inhibitors: A mechanistic exploration through pharmacophore based virtual screening, molecular docking coupled with Molecular dynamic simulation

Digital.CSIC. Repositorio Institucional del CSIC
  • Malik, Saima
  • Lodhi, Muhammad Arif
  • Ayaz, Sultan
  • Ullah, Zakir
Diabetes mellitus (DM) stands as a significant global health challenge, ranking third among causes of mortality worldwide. Despite extensive endeavors, effective treatments for diabetes remain elusive. Alpha-glucosidase, a pivotal enzyme in glycoprotein metabolism regulation, emerges as a promising therapeutic target for mitigating postprandial hyperglycemia, a hallmark of diabetes. In this study, we employed advanced computational methodologies to identify inhibitors of lysosomal α-glucosidase. Leveraging pharmacophore-based virtual screening of a vast library of drug-like molecules, we unearthed 161 potential inhibitors capable of binding within the enzyme's active pocket. Subsequent molecular docking simulations yielded five lead molecules exhibiting robust binding affinities and favorable interaction profiles with critical catalytic residues. Further analysis through molecular dynamics simulations provided crucial insights into the stability and conformational dynamics of the inhibitor-enzyme complexes. Notably, certain residues emerged as pivotal for the retention of inhibitors within the active site. Our findings underscore the potential of LIG1-LIG5 as promising inhibitors against lysosomal α-glucosidase, presenting novel avenues for the development of effective diabetes therapeutics. This research enriches our understanding of the molecular underpinnings of diabetes treatment, facilitating targeted drug development strategies in the quest for improved patient outcomes., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Exploring nitric acid's role in photo-catalytic conversion: Synergy with phosphorus corrole for enhanced mesitylene transformation

Digital.CSIC. Repositorio Institucional del CSIC
  • Zhan, Xuan
  • Ullah, Zakir
Nitric acid (HNO3) has garnered attention as a versatile acid reagent in laboratory and industrial settings, primarily known for its role in explosives and fertilizer production. Recent studies have explored its application in catalytic processes, particularly in electro- and photo-catalysis, including its involvement in nitrogen fixation and oxidation. This study investigates the photo-catalytic performance of HNO3 in the conversion of mesitylene to 3,5-dimethylbenzaldehyde, an industrially significant compound. Our results reveal successful conversion under irradiation conditions, with systematic optimizations indicating an optimal concentration of 0.2 M HNO3. Mechanistic studies employing scavenger assays suggest the involvement of hydroxyl radicals in the formation of aldehydes. Furthermore, synergistic effects between HNO3 and phosphorus corrole photosensitizers enhance catalytic performance. Subsequent optimization of reaction conditions yields a maximum yield of 45 % for 3,5-dimethylbenzaldehyde. Expansion of the scope to include toluene derivatives demonstrates varying yields, influenced by substituent effects. Notably, the combination of HNO3 with the corrole catalyst leads to improved yields compared to HNO3 alone. These findings underscore the potential of HNO3 as a photo-catalyst and highlight opportunities for novel catalyst design in practical applications., This work was supported by youth Program (2022A1515110577) funded by Guangdong Provincial Basic and Applied Basic Research Fund Project., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Battling hazardous gas molecules with kekulene surfaces: A computational study

Digital.CSIC. Repositorio Institucional del CSIC
  • Sattar, Fazli
  • Wang, Zhenzhen
  • Zhou, Xiaozhuang
  • Ullah, Zakir
A Density Functional Theory were used to investigate the interactions between kekulene and various noxious gases, including methane(CH4), carbon dioxide (CO2), hydrogen(H2), ammonia(NH3), and sulfur dioxide(SO2). The adsorption energies and bond distances were computed, indicating successful molecular interactions with kekulene, particularly notable in the exothermic nature of the adsorption process. Enthalpy calculations further confirmed the exothermic nature of the reactions, suggesting spontaneous adsorption. The analysis of frontier molecular orbitals revealed distinctive electronic characteristics, with HOMO-LUMO plots indicating a significant energy gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO). Chemical descriptors derived from these calculations provided insights into the reactivity and polarizability of the compounds. Furthermore, the molecular electrostatic potential (MEP) surface maps illustrated the electrostatic potential distribution, aiding in predicting the molecule's reactivity. Overall, the study highlights the potential of kekulene as a selective adsorbent for toxic gas (SO2), offering valuable insights into its chemical and electronic properties for various applications, particularly in environmental and industrial settings., This work was financially supported by Foundation of Yangtze Delta Region Institute (Huzhou) of UESTC (U032200124)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Inducing Efficient and Multiwavelength Circularly Polarized Emission From Perovskite Nanocrystals Using Chiral Metasurfaces

Digital.CSIC. Repositorio Institucional del CSIC
  • Fiuza-Maneiro, Nadesh
  • Mendoza Carreño, José
  • Gómez Graña, Sergio
  • Alonso Carmona, M. Isabel
  • Polavarapu, Lakshminarayana
  • Mihi, Agustín
Chiral nano-emitters have recently received great research attention due to their technological applications and the need for a fundamental scientific understanding of the structure-property nexus of these nanoscale materials. Lead halide perovskite nanocrystals (LHP NCs) with many interesting optical properties have anticipated great promise for generating chiral emission. However, inducing high anisotropy chiral emission from achiral perovskite NCs remains challenging. Although chiral ligands have been used to induce chirality, their anisotropy factors (glum) are low [10-3 to 10-2]. Herein, the generation of high anisotropy circularly polarized photoluminescence (CPL) from LHP NCs is demonstrated using chiral metasurfaces by depositing nanocrystals on top of prefabricated resonant photonic structures (2D gammadion arrays). This scalable approach results in CPL with glum to a record high of 0.56 for perovskite NCs. Furthermore, the differences between high-index dielectric chiral metasurfaces and metallic ones are explored for inducing chiral emission. More importantly, the generation of simultaneous multi-wavelength circularly polarized light is demonstrated by combining dielectric and metallic chiral metasurfaces., N.F.M. and J.M.C. contributed equally to this work. This work had received funding from the Spanish Agencia Estatal de Investigación (AEI/MCIN) through grants, PID2022-141956NB-I00 MCIN/AEI/10.13039/501100011033 (OUTLIGHT), and CEX2023-001263-S (Spanish Severo Ochoa Centre of Excellence program) and from the Generalitat de Catalunya (2021-SGR-00444). J.M.C. acknowledges an FPI fellowship (PRE2020-09411) from MICINN co-financed by the European Social Fund and the Ph.D. program in Materials Science from Universitat Autònoma de Barcelona UAB. L.P. acknowledges support from the Spanish Ministerio de Ciencia e Innovación through Ramón y Cajal grant (grant no. RYC2018-026103-I), the Spanish State Research Agency (grant nos. PID2020-117371RA-I00 and TED2021-131628A-I00), funded by MICIU/AEI/10.13039/501100011033 and European Union Next Generation EU/PRTR, and a grant from the Xunta de Galicia (grant no. ED431F2021/05). S.G.G. acknowledge support by the project CNS2022-135531 (funded by MICIU/AEI/10.13039/501100011033 and European Union Next Generation EU/PRTR). This research was also supported by the EIC PATHFINDER CHALLENGES project 101162112 (RADIANT), funded by the European Union. Funding for open access by the Universidade de Vigo/CISUG., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Promoting Polysulfide Redox Reactions through Electronic Spin Manipulation

Digital.CSIC. Repositorio Institucional del CSIC
  • Yu, Jing
  • Huang, Chen
  • Usoltsev, Oleg
  • Black, Ashley P.
  • Gupta, Kapil
  • Spadaro, Maria Chiara
  • Pinto Huguet, Ivan
  • Botifoll, Marc
  • Li, Canhuang
  • Herrero Martín, Javier
  • Zhou, Jinyuan
  • Ponrouch, Alexandre
  • Zhao, Ruirui
  • Balcells, Lluís
  • Zhang, Chao Yue
  • Cabot, Andreu
  • Arbiol, Jordi
Catalytic additives able to accelerate the lithium-sulfur redox reaction are a key component of sulfur cathodes in lithium-sulfur batteries (LSBs). Their design focuses on optimizing the charge distribution within the energy spectra, which involves refinement of the distribution and occupancy of the electronic density of states. Herein, beyond charge distribution, we explore the role of the electronic spin configuration on the polysulfide adsorption properties and catalytic activity of the additive. We showcase the importance of this electronic parameter by generating spin polarization through a defect engineering approach based on the introduction of Co vacancies on the surface of CoSe nanosheets. We show vacancies change the electron spin state distribution, increasing the number of unpaired electrons with aligned spins. This local electronic rearrangement enhances the polysulfide adsorption, reducing the activation energy of the Li-S redox reactions. As a result, more uniform nucleation and growth of Li2S and an accelerated liquid-solid conversion in LSB cathodes are obtained. These translate into LSB cathodes exhibiting capacities up to 1089 mA h g-1 at 1 C with 0.017% average capacity loss after 1500 cycles, and up to 5.2 mA h cm-2, with 0.16% decay per cycle after 200 cycles in high sulfur loading cells., This study is part of the Advanced Materials program and In-CAEM project, supported by MCIN with funding from the European Union Next Generation EU (PRTR-C17.I1) and by Generalitat de Catalunya. This work is in the framework of the Universitat Autònoma de Barcelona Materials Science PhD program. ICMAB-CSIC members thank the State Investigation Agency and Spanish Ministery of Science, Innovation and Universities through (PID2020-113805GB-I00) and OXISOT (PID2021-128410OB-I00). ICN2 acknowledges funding from grant IU16-014206 (METCAM-FIB) funded by the European Union through the European Regional Development Fund (ERDF), with the support of the Ministry of Research and Universities, Generalitat de Catalunya. ICN2 is a founding member of e-DREAM.(71) This work was financially supported by the SyDECat project from the Spanish MCIN/AEI/FEDER (PID2022-136883OB-C22), the 2BoSS project of the ERA-MIN3 program with the Spanish grant number PCI2022-132985/AEI/10.13039/501100011033, Generalitat de Catalunya 2021 SGR 01581 and 2021 SGR 00457 and European Union Next Generation EU/PRTR. IREC and ICN2 are both funded by the CERCA Program/Generalitat de Catalunya. The authors thank the support from the projects ENE2016-77798-C4-3-R and NANOGEN (PID2020-116093RB-C43), funded by MCIN/AEI/10.13039/501100011033/and by “ERDF A way of making Europe”, by the “European Union”. ICN2 and ICMAB acknowledge the support from the Severo Ochoa Programme (MINECO, grant no. CEX2021-001214-S and CEX2023-001263-S). A.P. acknowledges the funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant no. 715087)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




The general equation of δ direct methods and the novel SMAR algorithm residuals using the absolute value of ρ and the zero conversion of negative ripples

Digital.CSIC. Repositorio Institucional del CSIC
  • Rius, Jordi
"This paper is dedicated to the memory of Professor Carles Miravitlles"., The general equation δM(r) = ρ(r) + g(r) of the δ direct methods (δ-GEQ) is established which, when expressed in the form δM(r) - ρ(r) = g(r), is used in the SMAR phasing algorithm [Rius (2020). Acta Cryst A76, 489-493]. It is shown that SMAR is based on the alternating minimization of the two residuals Rρ(χ) = ∫V [ρ(χ) - ρ(Φ)sρ]2 dV and Rδ(Φ) = ∫V mρ[δM(χ) - ρ(Φ)sρ]2 dV in each iteration of the algorithm by maximizing the respective Sρ(Φ) and Sδ(Φ) sum functions. While Rρ(χ) converges to zero, Rδ(Φ) converges, as predicted by the theory, to a positive quantity. These two independent residuals combine δM and ρ each with |ρ| while keeping the same unknowns, leading to overdetermination for diffraction data extending to atomic resolution. At the beginning of a SMAR phase refinement, the zero part of the mρ mask [resulting from the zero conversion of the slightly negative ρ(Φ) values] occupies ∼50% of the unit-cell volume and increases by ∼5% when convergence is reached. The effects on the residuals of the two SMAR phase refinement modes, i.e. only using density functions (slow mode) supplemented by atomic constraints (fast mode), are discussed in detail. Due to its architecture, the SMAR algorithm is particularly well suited for Deep Learning. Another way of using δ-GEQ is by solving it in the form ρ(r) = δM(r) - g(r), which provides a simple new derivation of the already known δM tangent formula, the core of the δ recycling phasing algorithm [Rius (2012). Acta Cryst. A68, 399-400]. The nomenclature used here is: (i) Φ is the set of φ structure factor phases of ρ to be refined; (ii) δM(χ) = FT-1{c(|E| - 〈|E|〉)×exp(iα)} with χ = {α}, the set of phases of |ρ| and c = scaling constant; (iii) mρ = mask, being either 0 or 1; sρ is 1 or -1 depending on whether ρ(Φ) is positive or negative., The following funding is acknowledged: Agencia Estatal de Investigación (grant Nos. PID2021-124734OB-C22 and CEX2023-001263-S). The author acknowledges the support of the publication fee by the CSIC Open Access Publication Support Initiative through its Unit of Information Resources for Research (URICI)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Room temperature compressed air-stable conductive copper films for flexible electronics

Digital.CSIC. Repositorio Institucional del CSIC
  • Pereira, H. Jessica
  • Makarovsky, Oleg
  • Amabilino, David B.
  • Newton, Graham N.
The state-of-the-art technology of fabricating printed copper electronics is focussed largely on thermal sintering restricting transition towards heat sensitive flexible substrates. Herein we report a pioneering technology which eliminates the need for conventional sintering. Biopolymer-stabilised copper particles are prepared such that they can be compressed at room temperature to generate air-stable films with very low resistivities (2.05 – 2.33 × 10−8 Ω m at 20 °C). A linear positive correlation of resistivity with temperature verifies excellent metallic character and electron microscopy confirms the formation of films with low porosity (< 4.6%). An aqueous ink formulation is used to fabricate conductive patterns on filter paper, first using a fountain/dip pen and then printing to deposit more defined patterns (R < 2 Ω). The remarkable conductivity and stability of the films, coupled with the sustainability of the approach could precipitate a paradigm-shift in the use of copper inks for printable electronics., We thank the Propulsion Futures Beacon of Excellence at the University of Nottingham for funding and facilities. We thank the Schools of Chemistry and Physics, the Nanoscale and Microscale Research Centre (nmRC) of University of Nottingham and School of Electronics and Computer Science of University of Southampton for research facilities. The authors sincerely acknowledge, Dr. Craig Stoppiello and Dr. Long Jiang (XPS), Dr. Michael Fay (TEM), Dr. Tong Liu (elemental analysis) and Dr. Zhongnan Duan (MALDI-TOF-MS) for their support. HJP thanks University of Southampton for the award of an Anniversary Fellowship and funding., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Direct Synthesis of 2-Hydroxytrifluoroethylacetophenones via Organophotoredox-Mediated Net-Neutral Radical/Polar Crossover

Digital.CSIC. Repositorio Institucional del CSIC
  • Gallego Gamo, Albert
  • Sarró, Pau
  • Ji, Yingmin
  • Pleixats, Roser
  • Molins, Elies
  • Gimbert Suriñach, Carolina
  • Vallribera, Adelina
  • Granados, Albert
Alkene difunctionalization is a very attractive tool in synthetic organic chemistry. Herein, we disclose an operationally and practically simple method to access 2-hydroxytrifluoroethylacetophenones from styrene derivatives via photoredox catalysis. This light-mediated transformation promotes the generation of the 1-hydroxy-2,2,2-trifluoroethyl carbon-centered radical as key synthon, which undergoes Giese addition with styrenes followed by a Kornblum oxidation process. The presented method is not only mild and cost-effective, but also utilizes an organic photocatalyst and DMSO as oxidant. Experimental investigations support the operative mechanism via net-neutral radical/polar crossover., Support for this work under grants PID2021-124916NB-I00, RED2022-134287-T, RYC2019-027423-I, and PID2021-128496OB-I00, PID2021-124572OB-C32 from the MICINN (Spain) and 2021SGR00064 from AGAUR Generalitat de Catalunya are gratefully acknowledged., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Observation of Antiferroelectric Domain Walls in a Uniaxial Hyperferroelectric

Digital.CSIC. Repositorio Institucional del CSIC
  • Conroy, Michele
  • Småbråten, Didrik René
  • Ophus, Colin
  • Shapovalov, Konstantin
  • Ramasse, Quentin M.
  • Hunnestad, Kasper Aas
  • Selbach, Sverre M.
  • Aschauer, Ulrich
  • Moore, Kalani
  • Gregg, J Marty
  • Bangert, Ursel
  • Stengel, Massimiliano
  • Gruverman, Alexei
  • Meier, Dennis
Ferroelectric domain walls are a rich source of emergent electronic properties and unusual polar order. Recent studies show that the configuration of ferroelectric walls can go well beyond the conventional Ising-type structure. Néel-, Bloch-, and vortex-like polar patterns have been observed, displaying strong similarities with the spin textures at magnetic domain walls. Here, the discovery of antiferroelectric domain walls in the uniaxial ferroelectric Pb5Ge3O11 is reported. Highly mobile domain walls with an alternating displacement of Pb atoms are resolved, resulting in a cyclic 180° flip of dipole direction within the wall. Density functional theory calculations show that Pb5Ge3O11 is hyperferroelectric, allowing the system to overcome the depolarization fields that usually suppress the antiparallel ordering of dipoles along the longitudinal direction. Interestingly, the antiferroelectric walls observed under the electron beam are energetically more costly than basic head-to-head or tail-to-tail walls. The results suggest a new type of excited domain-wall state, expanding previous studies on ferroelectric domain walls into the realm of antiferroic phenomena., M.C. acknowledges funding from Science Foundation Ireland (SFI) Industry Fellowship (18/IF/6282), Royal Society Tata University Research Fellowship (URF\R1\201318), EPSRC NAME Programme Grant EP/V001914/1 and Royal Society Enhancement Award RF\ERE\210200EM1. The research by M.C., K.M., J.M.G., U.B., and A.G. was supported by the US-Ireland R&D Partnership Programme (grant no. USI 120), National Science Foundation (NSF) grant DMR-1709237 and Science Foundation Ireland (16/US/3344). D.R.S. and S.M.S. acknowledge the Research Council of Norway (FRINATEK project No. 275139/F20) for financial support. D.R.S. and U.A. acknowledge the Swiss National Science Foundation (Project No. 200021_178791) for financial support. Computational resources were provided by UNINETT Sigma2 (project no. NN9259K), and UBELIX (http://www.id.unibe.ch/hpc) – the HPC cluster at the University of Bern. C.O. acknowledges support from the DOE Early Career Research Program. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. SuperSTEM is the U.K. National Research Facility for Advanced Electron Microscopy, supported by the EPSRC through grant EP/W021080/1. M.S. and K.S. acknowledge support from Ministerio de Ciencia Y Innovación (MICINN-Spain) through Grant No. PID2019-108573GB-C22; from the State Investigation Agency through the Severo Ochoa Programme for Centres of Excellence in R&D (CEX2023-001263-S); from Generalitat de Catalunya (Grant No. 2021 SGR 01519); and from the European Research Council (Grant Agreement No. 724529). D.M. thanks NTNU for support through the Onsager Fellowship Program, the Outstanding Academic Fellow Program, and acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Program (Grant Agreement No. 863691). The Research Council of Norway (RCN) is acknowledged for the support to the Norwegian Micro- and Nano-Fabrication Facility, NorFab, project number 295864., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Deterministic grayscale nanotopography to engineer mobilities in strained MoS2 FETs

Digital.CSIC. Repositorio Institucional del CSIC
  • Liu, Xia
  • Erbas, Berke
  • Conde Rubio, Ana
  • Rivano, Norma
  • Wang, Zhenyu
  • Jiang, Jin
  • Bienz, Siiri
  • Kumar, Naresh
  • Sohier, Thibault
  • Penedo, Marcos
  • Banerjee, Mitali
  • Fantner, Georg
  • Zenobi, Renato
  • Marzari, Nicola
  • Kis, Andras
  • Boero, Giovanni
  • Brugger, Juergen
Field-effect transistors (FETs) based on two-dimensional materials (2DMs) with atomically thin channels have emerged as a promising platform for beyond-silicon electronics. However, low carrier mobility in 2DM transistors driven by phonon scattering remains a critical challenge. To address this issue, we propose the controlled introduction of localized tensile strain as an effective means to inhibit electron-phonon scattering in 2DM. Strain is achieved by conformally adhering the 2DM via van der Waals forces to a dielectric layer previously nanoengineered with a gray-tone topography. Our results show that monolayer MoS2 FETs under tensile strain achieve an 8-fold increase in on-state current, reaching mobilities of 185 cm²/Vs at room temperature, in good agreement with theoretical calculations. The present work on nanotopographic grayscale surface engineering and the use of high-quality dielectric materials has the potential to find application in the nanofabrication of photonic and nanoelectronic devices., The authors thank the Center of Micro/Nanotechnology (CMi) of EPFL for the AFM facility support. X.L., B.E., A.C., G.B., and J.B. acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Project “MEMS 4.0”, ERC-2016-ADG, grant agreement No. 742685), NFFA-Europe Pilot Project (the EU’s H2020 framework program for research and innovation, grant agreement No. 101007417). X.L. acknowledges fundings from the National Natural Science Foundation of China (No. 62274013) and the National Key Research and Development Program of China (No. 2023YFB3405600). M.B. acknowledges the support of SNSF Eccellenza grant No. PCEGP2_194528, and support from the QuantERA II Programme that has received funding from the European Union’s Horizon 2020 research and innovation program under Grant Agreement No 101017733. R.Z. acknowledges funding from the Swiss National Science Foundation through the NCCR MARVEL (project number 200021-143636) and the R’Equip program (grant number 206021-205312), as well as computational support from the Swiss National Supercomputing Centre. N.R. and N.M. acknowledge funding from the Swiss National Science Foundation (SNSF) and its National Centre of Competence in Research MARVEL on ‘Computational Design and Discovery of Novel Materials’ (grant number 182892). They also acknowledge computational support from the Swiss National Supercomputing Centre CSCS under project ID mr24. Z.W. and A.K. acknowledge financing from European Union’s Horizon 2020 research and innovation program under grant agreements 881603 (Graphene Flagship Core 3) and No 964735 (EXTREME-IR). G.F. and M.P. received funding through Innosuisse (AFM with PORT: Atomic force microscope with photothermal off-resonance tapping, grant number 7879, ext ref. 36938.1 IP-EE), FNS (Video-rate nanomechanical properties mapping using atomic force microscopy, grant number 7288, ext. ref. 200021_182562), H2020 (InCell - High speed AFM imaging of molecular processes inside living cellsInCell - High speed AFM imaging of molecular processes inside living cells, grant number 6823, ext ref. 773091, ETH Domain (An ecosystem for community driven scanning probe microscopy research and development, grant number 10126) and Eurostars (Correlated Analysis System for in-vivo Inspection of Semi-Conductor Process Wafers, grant number 9953, ext. ref. E!665 CAS-C)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Exploring ortho-dianthrylbenzenes for molecular solar thermal energy storage

Digital.CSIC. Repositorio Institucional del CSIC
  • Baggi, Nicolò
  • Muhammad, Lidiya M.
  • Liasi, Zacharias
  • Elholm, Jacob Lynge
  • Baronas, Paulius
  • Molins, Elies
  • Mikkelsen, Kurt V.
  • Moth-Poulsen, Kasper
Molecular solar thermal systems, which absorb light, store it, and release it as heat, have been extensively researched, yet many potential candidates remain unexplored. To expand this range, five specifically designed ortho-dianthrylbenzenes were investigated. Anthracene dimers have been underexplored due to issues like photooxidation and varying photodimerization efficiency. The presented systems address these challenges by aryl-linking two anthracene moieties, achieving photodimerization quantum yields ranging from 11.5% to 16% in mesitylene. The impact of donor or acceptor groups on energy storage time (9-37 years), energy storage density (0.14-0.2 MJ kg-1), and solar energy storage efficiency (0.38-0.66%) was evaluated. The experimental results, supported by density functional theory-based modeling, highlight the potential of anthracene-based photoswitches for molecular solar thermal applications and encourage further exploration of similar systems., Funding from the European Commission (H2020-FETPROACT-2019-951801; Molecular Solar Thermal Energy Storage Systems) and the European Research Council (ERC) under grant agreement CoG, PHOTHERM– 101002131 is acknowledged by the authors. The authors would like to also acknowledge the financial support from the Göran Gustafsson Foundation, the Swedish Research Council, the Spanish Ministry for Science and Innovation (project LIPCES, PID2021-123873NB-I00) and the Catalan Institute of Advanced Studies (ICREA). K. V. M. acknowledges the Danish Council for Independent Research, DFF-0136-00081B, DFF-10.46540/3103-00261B and the European Union's Horizon 2020 Framework Programme under grant agreement number 951801 for financial support. E. M. acknowledges financial support from the State Investigation Agency (PID2021-124572OB-C32), and through the Severo Ochoa Programme for Centres of Excellence in R&D (CEX2023-001263-S)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




The Role of Rare-Earth Atoms in the Anisotropy and Antiferromagnetic Exchange Coupling at a Hybrid Metal-Organic Interface

Digital.CSIC. Repositorio Institucional del CSIC
  • Blanco Rey, María
  • Castrillo, Rodrigo
  • Ali, Khadiza
  • Gargiani, Pierluigi
  • Ilyn, Maxim
  • Gastaldo, Michele
  • Paradinas, Markos
  • Valbuena, Miguel A.
  • Mugarza, Aitor
  • Ortega, J Enrique
  • Schiller, Frederik
  • Fernández, Laura
Main paper: 10 pages and 3 figures; Supplementary Material: 13 pages,
5 figures, Magnetic anisotropy and magnetic exchange interactions are crucial parameters that characterize the hybrid metal-organic interface, a key component of an organic spintronic device. It is shown that the incorporation of 4f RE atoms to hybrid metal-organic interfaces of CuPc/REAu2 type (RE = Gd, Ho) constitutes a feasible approach toward on-demand magnetic properties and functionalities. The GdAu2 and HoAu2 substrates differ in their magnetic anisotropy behavior. Remarkably, the HoAu2 surface promotes the inherent out-of-plane anisotropy of CuPc, owing to the match between the anisotropy axis of substrate and molecule. Furthermore, the presence of RE atoms leads to a spontaneous antiferromagnetic exchange coupling at the interface, induced by the 3d-4f superexchange interaction between the unpaired 3d electron of CuPc and the 4f electrons of the RE atoms. It is shown that 4f RE atoms with unquenched quantum orbital momentum ( L$L$ ), as it is the case of Ho, induce an anisotropic interfacial exchange coupling., This work was financially supported by the Spanish Ministerio de Ciencia e Innovación (grants No. PID2019-103910GB-I00, PID2019-107338RB-C65, PID2020-116093RB-C44, and PID2021-123776NB-C21, PID2022-137685NB-I00, PID2022-140845OB-C63, CEX2021-001214-S, and CEX2020-001039-S funded by MCIN/AEI/10.13039/501100011033/ and by “ESF investing in your future”), as well as the Department of Education, Universities and Research of the Basque Government (grants No. IT1591-22 and IT1527-22 and IKUR Quantum program) and the CERCA Programme/Generalitat de Catalunya and Diputación Foral de Gipuzkoa through the QUAMOS project within the Gipuzkoa Quantum program (DFG-QUAN-000029-01). L.F. acknowledges funding from the European Union's Horizon 2020 research and innovation programme through the Marie Skłodowska-Curie Grant Agreement MagicFACE No. 797109. Javier Fernández-Rodríguez is acknowledged for useful discussions. Computational resources were provided by DIPC., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Tuning plasmid DNA amounts for cost-effective transfections of mammalian cells: when less is more

Digital.CSIC. Repositorio Institucional del CSIC
  • Carreño, Aida
  • Guerrero Yagüe, Rubén
  • Casal, Enriqueta
  • Mendoza, Rosa
  • Corchero, José Luis
Transient gene expression (TGE) in mammalian cells is a well-known approach to the fast expression of recombinant proteins. The human cell line HEK (human embryonic kidney) 293F is widely used in this field, due to its adaptability to grow in suspension to high cell densities in serum-free media, amenability to transfection, and production of recombinant proteins in satisfactory quantities for functional and structural analysis. Amounts of plasmid DNA (pDNA) required in transfections for TGE remain high (usually 1 µg pDNA/mL, or even higher), representing a noticeable proportion of the overall cost. Thus, there is an economic need to reduce amounts of coding pDNA in TGE processes. In this work, amounts of both pDNA and transfecting agent used for TGE in HEK 293F cells have been explored in order to reduce them without compromising (or even improving) the productivity of the process in terms of protein yield. In our hands, minimal polyethyleneimine (PEI) cytotoxicity and optimum protein yields were obtained when transfecting at 0.5 µg pDNA/mL (equal to 0.5 µg pDNA/million cells) and a DNA-to-PEI ratio of 1:3, a trend confirmed for several unrelated recombinant proteins. Thus, carefully tuning pDNA and transfecting agent amounts not only reduces the economic costs but also results in higher recombinant protein yields. These results surely have a direct application and interest for the biopharmaceutical industry, always concerned in increasing productivity while decreasing economic costs. KEY POINTS: • Mammalian cells are widely used to produce recombinant proteins in short times. • Tuning DNA and transfecting agent are of great interest to optimize economic costs. • Reducing DNA and transfecting agent amounts result in higher protein yields., Open Access Funding provided by Universitat Autonoma de Barcelona. We acknowledge the financial support to our research in the field of production of recombinant proteins received from Instituto de Salud Carlos III, through “Acciones CIBER.” The Networking Research Center on Bioengineering, Biomaterials, and Nanomedicine (CIBER-BBN) is an initiative funded by the VI National R&D&I Plan 2008–2011, Iniciativa Ingenio 2010, Consolider Program, CIBER Actions and financed by the Instituto de Salud Carlos III with assistance from the European Regional Development Fund. The authors also appreciate the support of Spanish Ministerio de Ciencia, Innovación y Universidades, and Instituto de Salud Carlos III through the projects PI17/00553, PI17/00150, PI20/00770, and PI20/00623, co-funded by European Regional Development Fund (ERDF, “a way to make Europe”). The authors also acknowledge the financial support from Fundación Mutua Madrileña (FMMA) through project “Targeted therapy for selective elimination of metastatic stem cells CXCR4 + in endometrial cancer” (AP1666942017), from Asociación Española contra el cancer (AECC) through project “Development of an antitumor protein delivery system into ovarian cancer cells using the subcellular vault” (IDEAS18038BENI), from Agencia Nacional de Promoción Científica y Tecnológica (ANPCYT, Argentina) through grant PICT Start-Up (2018–00811), and from CIBER-BBN through the projects PEGLYSO 2, EXPLORE 3, and MANTRA 2. A.C. is supported by a predoctoral fellowship from Ministerio de Ciencia, Innovación y Universidades (PRE2019-089017)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Experimental and theoretical studies of the electronic transport of an extended curcuminoid in graphene nano-junctions

Digital.CSIC. Repositorio Institucional del CSIC
  • Cardona, Teresa
  • Baum, Thomas Y.
  • Zaffino, Rossella
  • Herrera, Daniel
  • Pfattner, Raphael
  • Gómez Coca, Silvia
  • Ruiz, Eliseo
  • González Campo, Arántzazu
  • Zant, Herre S.J. van der
  • Aliaga Alcalde, Núria
Exploiting the potential of curcuminoids (CCMoids) as molecular platforms, a new 3.53 nm extended system (pyACCMoid, 2) has been designed in two steps by reacting a CCMoid with amino-terminal groups (NH2-CCMoid, 1, of 1.79 nm length) with polycyclic aromatic hydrocarbon (PAH) aldehydes. CCMoid 2 contains pyrene units at both ends as anchoring groups to optimize its trapping in graphene nano-junctions created by feedback-controlled electro-burning. The measured I-V characteristics show gate-dependent behaviour at room temperature and 10 K, with increased conductance values compared to shorter CCMoids previously reported, and in agreement with DFT calculations. Our results show that the adjusted molecular design improves the conductance, as system 2 separates the conductive backbone from the anchor groups, which tend to adopt a planar configuration upon contact with the graphene electrodes. DFT calculations using Green functions of a set of different molecular conformations of 2 on graphene electrodes show a direct relationship between the units (e.g. pyrene, amide, etc.), in the molecule, through which electrons are injected and the conductance values; where the size of the spacing between the graphene electrodes contributes but is not the dominant factor, and thus, counter-intuitively the smallest spacing gives one of the lowest conductance values., This work has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 R&D program (ERC-724981) and grant no. 863098 (SPRING). This work was also supported by the projects PID2019-108794GBI00, TED2021-129593B-I00 and PID2021-122464NB-I00 funded by MCIN/AEI/10.13039/501100011033 from the Ministerio de Ciencia e Innovación. R. P. acknowledges support from the Ramón y Cajal Fellowship (Ref. RyC2019-028474-I). E. R. thanks Generalitat de Catalunya for an ICREA Academia award and 2021-SGR-00286 grant, Spanish Ministry Science for a Maria de Maeztu excellence grant (CEX2021-001202-M), and BSC for computational resources. The CSIC authors acknowledge the financial support from the Spanish Ministry Science, through the “Severo Ochoa” Programme for Centres of Excellence (MATRANS42, CEX2023-001263-S)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Twisto-photonics in two-dimensional materials: A comprehensive review

Digital.CSIC. Repositorio Institucional del CSIC
  • Zhou, Renlong
  • Habib, Muhammad
  • Iqbal, Muhammad Faisal
  • Hussain, Naveed
  • Farooq, Sajid
  • Haleem, Yasir A.
  • Ali, Faizan
  • Ullah, Kaleem
Twisted two-dimensional materials (t2DMs) such as graphene and black phosphorus are transforming the field of photonics, serving as a promising platform for the development of advanced devices that manipulate light. These materials possess multiple photonic properties that are determined by their twist angles. This article explores the profound impact of twist angles on various photonic phenomena, including nonlinear optical responses, optical absorption, plasmonics, and the influence of chirality in t2DMs. We delve into cutting-edge developments explained through Raman spectroscopy and the intriguing world of moiré excitons, as revealed through photoluminescence studies. As we explore device applications, we highlight groundbreaking advancements in photodetection, with a brief look into emerging technologies such as single-photon detectors, ultrafast modulators, light-emitting diodes, and interlayer exciton lasers. Our study extends to depict the promising future of t2DMs, emphasizing their prospective integration with other photonic systems and the discovery of novel optical phenomena in the domain of photonics. This review serves as a comprehensive guide to the dynamic field of photonics in t2DMs, highlighting current achievements and future prospects., The authors acknowledge the support provided by the Guangdong Basic and Applied Basic Research Foundation (2020A1515110488) and the Scientific Key Research Fund of Guangdong Provincial Education Department (2019KZDXM061, 2019KQNCX099, 2020ZDZX2059, 2021ZDZX1038)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S)., Peer reviewed




Corrole–chelated phosphorus complex: enabling dual C–H chlorination and H₂O₂ generation

Digital.CSIC. Repositorio Institucional del CSIC
  • Zhan, Xuan
  • Kim, Donghyeon
  • Ullah, Zakir
  • Churchill, David G.
Corroles, despite their highly tunable and excellent photophysical and electrochemical properties, have rarely been explored as mainstream photocatalytic photosensitizers. Our study introduces a novel application of the highly oxidizing penta–CF3 substituted phosphorus corrole, P–(CF3)5, which has shown remarkable efficacy in the chlorination of phenol and related natural compounds (the beta 2, 3, 8, 17, 18-substituted isomer: 2,3,8,17,18–pentatrifluoromethyl–(5,10,15–tris(pentafluorophenyl) corrole phosphorus (V) difluoride). Here, we report the first case of the simultaneous photocatalytic chlorination of phenol or toluene and H2O2 formation, with the latter achieving a notable rate of > 7 mM/g/h under ambient conditions. Notably, the oxidation of toluene predominantly yields benzaldehyde over benzyl chloride. The H2O2 formation can be finely tuned by adjusting the water/acetonitrile ratio and acid concentration. Comprehensive experimental and theoretical (DFT) investigations were conducted to elucidate the underlying mechanisms of both chlorination and oxidation. This dual–function catalytic process not only enhances reaction efficiency but also underscores the potential of corrole–based catalysts in advancing sustainable and green chemical methodologies., This work was supported by youth Program (2022A1515110577) funded by Guangdong Provincial Basic and Applied Basic Research Fund Project. D. G. C. acknowledges support from KAIST and grant NRF–2021R1F1A104657613., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




3D Printing as a Strategy to Scale-Up Biohybrid Hydrogels for T Cell Manufacture

Digital.CSIC. Repositorio Institucional del CSIC
  • Pérez Del Río, Eduardo
  • Rey Vinolas, Sergi
  • Santos, Fabião
  • Castellote Borrell, Miquel
  • Merlina, Francesca
  • Veciana, Jaume
  • Ratera, Immaculada
  • Mateos Timoneda, Miguel A.
  • Engel, Elisabeth
  • Guasch, Judith
The emergence of cellular immunotherapy treatments is introducing more efficient strategies to combat cancer as well as autoimmune and infectious diseases. However, the cellular manufacturing procedures associated with these therapies remain costly and time-consuming, thus limiting their applicability. Recently, lymph-node-inspired PEG-heparin hydrogels have been demonstrated to improve primary human T cell culture at the laboratory scale. To go one step further in their clinical applicability, we assessed their scalability, which was successfully achieved by 3D printing. Thus, we were able to improve primary human T cell infiltration in the biohybrid PEG-heparin hydrogels, as well as increase nutrient, waste, and gas transport, resulting in higher primary human T cell proliferation rates while maintaining the phenotype. Thus, we moved one step further toward meeting the requirements needed to improve the manufacture of the cellular products used in cellular immunotherapies., This research was funded by the Spanish Ministry of Science and Innovation (PID2020-115296RA-I00; PID2019-105622RB-I00; PID2021-128412OB-I00 European Union NextGenerationEU/PRTR, and the “Ramón y Cajal” program (RYC-2017-22614)) as well as the Generalitat de Catalunya (SGRCat 2021-00438; 2017-SGR-359; Tecnologies Emergents program of the General Directorate for Research – Nr. 001-P-001646, cofunded with FEDER Operational Program of Catalonia 2014–2020). The work was also supported by the Max Planck Society through the Max Planck Partner Group “Dynamic Biomimetics for Cancer Immunotherapy” in collaboration with the Max Planck Institute for Medical Research (Heidelberg, Germany). The authors are grateful for the financial support received from Instituto de Salud Carlos III through Consorcio Centro de Investigación Biomédica en Red (CIBER) with the project “Gels4ACT” (Nr. BBN20PIV02). This research was also supported by the European Union’s Horizon 2020 research and innovation program H2020-MSCA-COFUND-2016 (DOC-FAM, grant agreement Nr. 754397). The authors acknowledge financial support from the Spanish Ministry of Science and Innovation through the “Severo Ochoa” Program for Centres of Excellence in R&D (CEX2023-001263-S, CEX2019-000917-S and CEX2018-000789-S)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).
With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Discrete versus polymeric structures of coordination compounds of copper(II) with (pyridin-2-yl)methylenenicotinohydrazide and a library of dicarboxylic acids

Digital.CSIC. Repositorio Institucional del CSIC
  • Benito, Mónica
  • Mahmoudi, Ghodrat
  • Molins, Elies
  • Zangrando, Ennio
  • Servati Gargari, Masoumeh
  • Frontera, Antonio
  • Safin, Damir A.
A series of copper(II) discrete and polymeric coordination compounds, namely [{CuL(H2O)}2(fum)] (1), [{CuL(H2O)}2(mes)] (2), [Cu2L2(glu)]n·2n(H2O) (3·2n(H2O)) and [Cu3L2(adi)2]n (4) were fabricated from (pyridin-2-yl)methylenenicotinohydrazide (HL) and a library of dicarboxylic acids, namely fumaric acid (H2fum), mesaconic acid (H2mes), glutaric acid (H2glu) and adipic acid (H2adi), using evaporative crystallization, grinding and slurry synthesis methods. The obtained coordination compounds have been fully characterized by single crystal X-ray diffraction revealing different types of complexes depending on the linker length, viz. from dinuclear complexes for the shorter linkers (fumaric and mesaconic acids) to 1D and 2D coordination polymers for longer glutaric and adipic acids. Thermal stability and spectroscopic features (FTIR and diffuse reflectance) of complexes were also studied. For the nonpolymeric compounds 1 and 2, the supramolecular assemblies driven by a combination of antiparallel π-stacking and hydrogen bonding interactions have been studied and compared using DFT calculations, MEP surface analysis and a combination of QTAIM and NCIplot computational tools., M. Benito and E. Molins acknowledge financial support from the State Investigation Agency, through the Severo Ochoa Programme for Centres of Excellence (projects CEX2019-00917-S and CEX2023-001263-S). M. Benito and E. Molins also thank the X-ray diffraction, thermal analysis and spectroscopic services from the ICMAB. This research was funded by the MICIU/AEI of Spain (project PID2021-1245720B-C32 and PID2020-115637GB-I00)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).
With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Two-way photoswitching norbornadiene derivatives for solar energy storage

Digital.CSIC. Repositorio Institucional del CSIC
  • Fei, Liang
  • Hölzel, Helen
  • Wang, Zhihang
  • Hillers-Bendtsen, Andreas Erbs
  • Aslam, Adil S.
  • Shamsabadi, Monika
  • Tan, Jialing
  • Mikkelsen, Kurt V.
  • Wang, Chaoxia
  • Moth-Poulsen, Kasper
Molecular photoswitches of norbornadiene (NBD) derivatives have been effectively applied in molecular solar-thermal energy storage (MOST) by photoisomerization of NBD to a quadricyclane (QC) state. However, a challenge of the NBD-based MOST system is the lack of a reversible two-way photoswitching process, limiting conversion from QC to thermal and catalytic methods. Here we design a series of NBD derivatives with a combination of acceptor and donor units to achieve two-way photoswitching, which can optically release energy by back-conversion from QC to NBD. Highly efficient photoconversion yields from NBD to QC and QC to NBD are up to 99% and 82%, respectively. The energy storage density of two-way photoswitching NBD is up to 312 J g-1 and optically controlled two-way photoswitching devices are demonstrated for the first time both in flow and in thin films, which illustrate a promising approach for fast and robust energy release in both solution and solid state., The authors acknowledge financial support from the European Commission (H2020-FETPROACT-2019-951801; Molecular Solar-Thermal Energy Storage Systems), the European Research Council (ERC) under grant agreement CoG, PHOTHERM – 101002131, the Göran Gustafsson Foundation, the Swedish Research Council, the Catalan Institute of Advanced Studies (ICREA), the National Natural Science Foundation of China (21975107), and the China Scholarship Council (202006790096)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Metal Propionate Solutions for High-Throughput Liquid-Assisted Manufacturing of Superconducting REBa2Cu3O7-δ (RE = Y, Gd, Sm, and Yb) Films

Digital.CSIC. Repositorio Institucional del CSIC
  • Saltarelli, Lavinia
  • Sanchez Rodríguez, Daniel
  • Gupta, Kapil
  • Kethamkuzhi, Aiswarya
  • Farjas, Jordi
  • Molins, Elies
  • Yáñez, Ramón
  • Ricart, Susagna
  • Obradors, Xavier
  • Puig Molina, Teresa
The cost-effective synthesis of a series of metal propionate powders (copper, yttrium, barium, samarium, gadolinium, and ytterbium) is developed through single chemical reactions resulting in five novel crystalline forms. These complexes are valuable precursors for the preparation of epitaxial REBa2Cu3O7-δ (REBCO) superconducting films (here, RE = Y, Sm, Gd, and Yb) through the innovative transient liquid-assisted growth (TLAG) process based on chemical solution deposition (CSD). TLAG-CSD shows impressive results with YBa2Cu3O7-δ (YBCO), obtaining critical current densities of 2.6 MA/cm2 (77 K) on 500 nm films at unprecedented growth rates (50-2000 nm/s), boosting unprecedented high-throughput industrial production. With a cardinal concern on designing the pyrolysis toward optimal nanocrystalline films for TLAG, an analysis of the thermal behavior of the synthesized precursors is essential. Decomposition pathways for each metal propionate are established, and compatibility with TLAG-CSD is corroborated. Metal-organic solutions for these REBCO systems are successfully prepared, and their rheological properties and thermal behavior are analyzed. This work demonstrates homogeneous nanocrystalline films through propionate-based REBCO precursor solutions, including several rare-earth ions, which display exemplary chemical and microstructural characteristics crucial for TLAG, and provides a base for a wide variety of CSD-based functional oxides., Authors acknowledge the European Research Council for the ULTRASUPERTAPE project (ERC-2014-ADG-669504), IMPACT project (ERC-2019-PoC-8749), SMS-INKS (ERC-2022-PoC-101081998), and EU COST actions OPERA (CA20116) and SUPERQUMAP (CA-21144). Also acknowledged is the financial support from the Spanish Ministry of Science and Innovation and the European Regional Development Fund, MCIU/AEI/FEDER for SUPERENERTECH (PID2021-127297OB-C21), “Severo Ochoa” Programs for Centers of Excellence in R&D (FUNFUTURE CEX2019-000917-S and Matrans42 CEX2023-001263-S), and HTS-JOINTS (PDC2022-133208-I00), PTI+ TransEner CSIC program for Spanish NGEU (Regulation (EU) 2020/2094). They also thank the Catalan Government for 2021 SGR 00440. L.S. and A.K. acknowledge financial support from the Spanish Ministry of Science, Innovation, and Universities through the FPI grant PRE2019-090621 and PRE2020-091817, respectively. D.S.R. acknowledges the support received from the Beatriu de Pinós Programme and the Ministry of Research and Universities of the Government of Catalonia (Fellowship BP00069). Authors thank the Scientific Services at ICMAB, ICN2 Electron Microscopy Division, and Scientific Services at the University of Girona. Authors acknowledge the use of instrumentation as well as the technical advice provided by the Joint Electron Microscopy Center at ALBA (JEMCA) and funding from Grant IU16-014206 (METCAM-FIB) to ICN2 funded by the European Union through the European Regional Development Fund (ERDF), with the support of the Ministry of Research and Universities, Generalitat de Catalunya. Part of the content of this manuscript is object of a European patent, application no. PCT/EP2023/070988 filed on 28/07/2023., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).
With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Induced electric wireless effects on energy storage: Bipolar electrochemistry effects on Cu/Zn batteries performance

Digital.CSIC. Repositorio Institucional del CSIC
  • Mosqueda, Marc
  • Flox, Cristina
  • Bengoa, Leandro N.
  • Goñi, Sandro M.
  • Casañ Pastor, Nieves
Immersed conducting materials in an electrolyte undergo polarization in presence of electric fields, resulting in a dipole where opposite poles of the material become an anode and cathode, where electrochemical reactions may occur at sufficiently induced potentials. Such induction phenomena lower significantly the resistance of the electrochemical cell. This work shows how in a Cu/Zn battery, it also yields lower overpotentials, and enhanced charge capacity and power, especially at high currents. The outcome of such bipolar electrochemistry, depends on the specific configuration of the bipolar electrodes within the electric field, and the possible reactions at the bipolar electrode for the specific redox system chosen. For the largest induced dipole tested, specific capacities may be increased by 40 % and volumetric capacities may double. It is of great significance that, with appropriate configurations, the capacity of a specific battery may be greatly enhanced, allowing also to reduce the number of cells in a stack to maintain the same performance., The authors thank financing from the Spanish Research Agency (AEI) through Grants PID2021-123276OB-I0, Severo Ochoa program CEX2023-001263-S and CEX2021-001214-S and European Commission under the grant MSCA-IF-EF-SE (101026162). This work has been carried out in the framework of the PhD program in Materials Science at the Autonomous University of Barcelona., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Photon upconversion crystals doped bacterial cellulose composite films as recyclable photonic bioplastics

Digital.CSIC. Repositorio Institucional del CSIC
  • Bharmoria, Pankaj
  • Naimovičius, Lukas
  • Abol-Fotouh, Deyaa
  • Miroshnichenko, Mila
  • Lekavičius, Justas
  • Luca, Gabriele de
  • Saeed, Umair
  • Kazlauskas, Karolis
  • Candau, Nicolas
  • Baronas, Paulius
  • Roig Serra, Anna
  • Moth-Poulsen, Kasper
Biopolymers currently utilized as substitutes for synthetic polymers in photonics applications are predominantly confined to linear optical color responses. Herein we expand their applications in non-linear optics by integrating with triplet-triplet annihilation photon upconversion crystals. A photon upconverting biomaterial is prepared by cultivating Pd(II) meso-tetraphenyl tetrabenzoporphine: 9,10-diphenyl anthracene (sensitizer: annihilator) crystals on bacterial cellulose hydrogel that serves both as host and template for the crystallization of photon upconversion chromophores. Coating with gelatin improves the material's optical transparency by adjusting the refractive indices. The prepared material shows an upconversion of 633 nm red light to 443 nm blue light, indicated by quadratic to linear dependence on excitation power density (non-linearly). Notably, components of this material are physically dis-assembled to retrieve 66 ± 1% of annihilator, at the end of life. Whereas, the residual clean biomass is subjected to biodegradation, showcasing the sustainability of the developed photonics material., This work was developed within the scope of the La-Caixa Junior Research Leadership-Post Doctoral Project PHOLCEB (ID: 100010434, fellowship code: LCF/BQ/P122/11910023). P.B. and M.M. acknowledge La-Caixa Foundation and the State Investigation Agency, through the Severo Ochoa Program for Centres of Excellence in R&D (CEX2023-001263-S) and Project PID2021-123873NB-I00 for financial support. K.M.P. acknowledges funding from the European Research Council (No. 101002131), the Swedish Energy Agency, the Göran Gustafsson Foundation, the Swedish Research Council, Swedish Research Council Formas, the European Research Council (ERC) under Grant Agreement CoG, PHOTHERM—101002131, the Catalan Institute of Advanced Studies (ICREA) and the European Union’s Horizon 2020 Framework Program under Grant Agreement No. 951801. L.N. acknowledges Erasmus+ Traineeship Program. J.L. and K.K. acknowledge the “Universities’ Excellence Initiative” program by the Ministry of Education, Science and Sports of the Republic of Lithuania under the agreement with the Research Council of Lithuania (Project No. S-A-UEI-23-6). A.R. acknowledges Grants PID2021-122645OB-I00 and CEX2019-000917 (“Severo Ochoa” Program for Center of Excellence in R&D) funded by MCIN/AEI/10.13039/501100011033 and by FEDER, “A way of making Europe”, and The Generalitat de Catalunya with Grant No. 2021SGR00446. N.C. acknowledges the group eb-POLICOM/Polímers i Compòsits Ecològics i Biodegradables, a research group of the Generalitat de Catalunya (Grant 2021 SGR 01042). D.A.F. is grateful to the Egyptian Ministry of Higher Education and Scientific Research for his post-doctoral grant. G.D.L. acknowledges funding from the Grant RYC2021-032524-I funded by MCIN/AEI/10.13039/501100011033 and by “European Union NextGenerationEU”/PRTR. G.D.L and U.S. acknowledge Prof. G. Catalan for the use of the LCR meter., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




A single nanophotonic platform for producing circularly polarized white light from non-chiral emitters

Digital.CSIC. Repositorio Institucional del CSIC
  • Mendoza Carreño, José
  • Bertucci, Simone
  • Garbarino, Mauro
  • Cirignano, Matilde
  • Fiorito, Sergio
  • Lova, Paola
  • Garriga Bacardi, Miquel
  • Alonso Carmona, M. Isabel
  • Stasio, Francesco di
  • Mihi, Agustín
Direct manipulation of light spin-angular momentum is desired in optoelectronic applications such as, displays, telecommunications, or imaging. Generating polarized light from luminophores avoids using optical components that cause brightness losses and hamper on-chip integration of light sources. Endowing chirality to achiral emitters for direct generation of polarized light benefits from existing materials and can be achieved by chiral nanophotonics. However, most chiral nanostructures operate in narrow wavelength ranges and involve nanofabrication processes incompatible with high-throughput production. Here, a single nanophotonic architecture is designed to sustain chiroptical resonances along the visible spectrum. This platform, fabricated with scalable soft-nanoimprint lithography transfers its chirality to conventional emitters (CdSe/CdS nanoplatelets, CdSe/CdS quantum dots, CsPbBr3, CsPbI3 perovskite nanocrystals and F8BT) placed atop, achieving a high dissymmetry emission factor (glum > 1). The dynamics study suggests enhanced out-coupling efficiency for one helicity by the photonic structure. Finally, a white light-emitting blend containing different emitters shows simultaneous dissymmetric emission values along the visible spectrum with this chiral nanophotonic platform., This work has received funding from the Spanish Agencia Estatal de Investigación (AEI/MCIN) through grants, PID2022-141956NB-I00 MCIN/AEI/10.13039/501100011033(OUTLIGHT), and CEX2023-001263-S (Spanish Severo Ochoa Centre of Excellence program) and from the Generalitat de Catalunya (2021-SGR-00444). This research was also supported by the EIC PATHFINDER CHALLENGES project 101162112 (RADIANT), funded by the European Union. J.M.C. acknowledges an FPI fellowship (PRE2020-09411) from MICINN co-financed by the European Social Fund and the Ph.D. program in Materials Science from Universitat Autònoma de Barcelona UAB. S.B., M.C., S.F., and F.D.S. acknowledge support by the European Research Council via the ERC-StG “NANOLED” (Grant 851794). M.G. and F.D.S. acknowledge support by the European Innovation Council via the Pathfinder OPEN “TWISTEDNANO” (Grant 101046424). S.B. also acknowledges Dorwal Marchelli for his insight on spectroscopy measurements and Simone Lauciello for the HR-SEM images., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




2024 roadmap for sustainable batteries

Digital.CSIC. Repositorio Institucional del CSIC
  • Titirici, Magda
  • Johansson, Patrik
  • Crespo Ribadeneyra, Maria
  • Au, Heather
  • Innocenti, Alessandro
  • Passerini, Stefano
  • Petavratzi, Evi
  • Lusty, Paul
  • Tidblad, Annika Ahlberg
  • Naylor, Andrew J.
  • Younesi, Reza
  • Chart, Yvonne A.
  • Aspinall, Jack
  • Pasta, Mauro
  • Orive, Joseba
  • Babulal, Lakshmipriya Musuvadhi
  • Reynaud, Marine
  • Latham, Kenneth G.
  • Hosaka, Tomooki
  • Komaba, Shinichi
  • Bitenc, Jan
  • Ponrouch, Alexandre
  • Zhang, Heng
  • Armand, Michel
  • Kerr, Robert
  • Howlett, Patrick C.
  • Forsyth, Maria
  • Brown, John
  • Grimaud, Alexis
  • Vilkman, Marja
  • Dermenci, Kamil Burak
  • Mousavihashemi, Seyedabolfazl
  • Berecibar, Maitane
  • Marshall, Jean E.
  • McElroy, Con Robert
  • Kendrick, Emma
  • Safdar, Tayeba
  • Huang, Chun
  • Zanotto, Franco M.
  • Troncoso, Javier F.
  • Domínguez, Diana Zapata
  • Alabdali, Mohammed
  • Vijay, Utkarsh
  • Franco, Alejandro A.
  • Pazhaniswamy, Sivaraj
  • Grant, Patrick S.
  • López Guzman, Stiven
  • Fehse, Marcus
  • Galceran, Montserrat
  • Antuñano, Néstor
Modern batteries are highly complex devices. The cells contain many components—which in turn all have many variations, both in terms of chemistry and physical properties. A few examples: the active materials making the electrodes are coated on current collectors using solvents, binders and additives; the multicomponent electrolyte, contains salts, solvents, and additives; the electrolyte can also be a solid ceramic, polymer or a glass material; batteries also contain a separator, which can be made of glass fibres, polymeric, ceramic, composite, etc. Moving up in scale all these components are assembled in cells of different formats and geometries, coin cells and Swagelok cells for funamental testing and understanding, and pouch, prismatic and cylindrical cells for application. Given this complexity dictated by so many components and variations, there is no wonder that addressing the crucial issue of true sustainability is an extremely challenging task. How can we make sure that each component is sustainable? How can the performance can be delivered using more sustainable battery components? What actions do we need to take to address battery sustainability properly? How do we actually qualify and quantify the sustainability in the best way possible? And perhaps most importantly; how can we all work—academia and battery industry together—to enable the latter to manufacture more sustainable batteries for a truly cleaner future? This Roadmap assembles views from experts from academia, industry, research institutes, and other organisations on how we could and should achieve a more sustainable battery future. The palette has many colours: it discusses the very definition of a sustainable battery, the need for diversification beyond lithium-ion batteries (LIBs), the importance of sustainability assessments, the threat of scarcity of raw materials and the possible impact on future manufacturing of LIBs, the possibility of more sustainable cells by electrode and electrolyte chemistries as well as manufacturing, the important role of new battery chemistries, the crucial role of AI and automation in the discovery of the truly sustainable batteries of the future and the importance of developimg a circular battery economy., H A would like to thank the Faraday Institution's LiSTAR project (EP/S003053/1, Grant FIRG014) for funding.
The authors acknowledge the EU's Horizon 2020 Research and Innovation Programme under Marie Skłodowska-Curie Grant Agreement 860403 'POLYSTORAGE' for the funding, as well as the Helmholtz Association basic funding.
The work in this paper was funded by the UKRI Interdisciplinary Circular Economy Centre for Technology Metals (Met4Tech) (EP/V011855/1) project.
This paper has been produced as an activity within Batteries Sweden (BASE), a Centre of Excellence co-funded by Sweden's Innovation Agency (Vinnova), the industry and the academy.
Y A C, J A, and M P acknowledge support by the Faraday Institution [Grant Numbers FIRG056 and FIRG058].
The authors acknowledge funding from MCIN/AEI/10.13039/501100011033 through the project ION-SELF ref. PID2019-106519RB-I00, as well as the Spanish Ministerio de Industria, Comercio y Turismo and the European Union—Next Generation EU for their financial support through the project VEC-020100-2022-127/PP27.
K G L acknowledges the European Research Council under the Horizon 2020 framework for the Marie Curie Research Fellowship (888124) through the project HYBRIDFLEX.
The authors thank the JSPS KAKENHI (Grant Nos. JP20H02849, JP21K20561, and JP22K14772),the MEXT Program: Data Creation and Utilization Type Materials Research and Development Project (JPMXP1122712807), and JST-CREST (Grant No. JPMJCR21O6) for financial support.
Funding from the European Research Council is acknowledged: ERC-2022-CoG, MULTIMETALBAT, Grant agreement No. 101089281. A P is grateful to the Spanish Agencia Estatal de Investigación Severo Ochoa Programme for Centres of Excellence in R&D (CEX2023-001263-S). J B would like to acknowledge financial support of Slovenian Research Agency through research programme P2-0423 and research Projects J2-4462 and N2-0279.
The authors acknowledge the financially supported by the National Natural Science Foundation of China (Nos. 52203223 and 22279037) and the Fundamental Research Funds for Central Universities, HUST (2020kfyXJJS095).
J B as a part of the DESTINY PhD programme acknowledges funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowská–Curie Grant Agreement No: 945357.
The authors are grateful to the UK Faraday Institution for financial support through grant SOLBAT—next generation solid state batteries [FIRG066].
This work has received funding from the European Union's Horizon 2020 research and innovation programme under Grant Agreements 957225 (BAT4EVER) and 957202 (HIDDEN). The authors want to thank the Battery 2030+ initiative (Grant Agreement No. 957213) for enabling the collaboration.
The authors would like to thank the Faraday Institution ReLiB project (Grant Codes FIRG005, FIRG027 and FIRG057) and UKRI Faraday Battery Challenge project 'Reclamation and Re-manufacture of lithium ion batteries,' Reference Number 104425 and The Faraday Institution. Manufacturing of Advanced Electrodes with Green Solvents—MAEGS, FIRG040.
This work was carried out with the support of the Faraday Institution (FIRG060, FIRG066), the Faraday Institution Industry Fellowship (FIIF015), the Faraday Institution Training Grant (FITG034), the ERC Starting Grant (converted to UKRI funding EP/Y009908/1), and the Imperial College London UKRI Impact Acceleration Account (EP/X52556X/1).
A A F and D Z D acknowledge the European Union's Horizon 2020 research and innovation program for the funding support through the European Research Council (Grant Agreement 772873, 'ARTISTIC' project). F M Z and A A F acknowledge the European Union's Horizon Europe research and innovation programme under Grant Agreement No. 101069686 (PULSELiON). M A, U V, and A A F as a part of the DESTINY PhD programme acknowledge funding from the European Union's Horizon2020 research and innovation programme under the Marie Skłodowska–Curie Actions COFUND—Grant Agreement No: 945357. M A and A A F also acknowledge the support of Umicore as part of DESTINY. A A F acknowledges the Institut Universitaire de France for their support. Some of the icons used in figure 23 are originated (free to use) from freepik.com.
The European Union's Horizon Europe research and innovation programme is acknowledged for funding the project HighSpin (GA No. 101069508) and the associated PhD of S L., Peer reviewed




A Comprehensive Study on the Parameters Affecting Magnesium Plating/Stripping Kinetics in Rechargeable Mg Batteries

Digital.CSIC. Repositorio Institucional del CSIC
  • Radi, Muath
  • Purkait, Taniya
  • Tchitchekova, Deyana S.
  • Goñi, Alejandro R.
  • Markowski, Robert
  • Bodin, Charlotte
  • Courrèges, Cécile
  • Dedryvère, Rémi
  • Ponrouch, Alexandre
Mg metal anode-based battery is a more sustainable, lower cost, and higher energy density alternative to Li-ion. However, this battery chemistry also faces several challenges associated with the high charge density of Mg2+, including achieving high reversibility and low voltage hysteresis for Mg metal plating/stripping. While significant improvements are achieved in last decades, they involve rather complex electrolyte formulations and/or Mg salts difficult to produce, and the use of unpractical substrates such as platinum. Here, significant improvement in terms of Mg plating kinetics is achieved in electrolytes containing commercial magnesium bis(trifluoromethanesulfonyl)imide salt (Mg(TFSI)2) by using titanium substrate with similar crystal structure and lattice parameter as Mg leading to lower nucleation overpotential. Low salt concentration electrolyte and addition of dibutyl magnesium (Mg(butyl)2) also enable the formation of thinner interphase, richer in solvent based decomposition products, further improving Mg plating kinetics. This work highlights the complex role of Mg(butyl)2, often considered as a simple drying agent, and how it impacts ion solvation favoring the mobility of electroactive cationic species, paving the way toward better electrolyte design with improved cation transference number., M.R. and T.P. contributed equally to this work. A.P. gratefully acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement No. 101089281). A.P., T.P., D.S.T. and A.R.G. acknowledge the Spanish Agencia Estatal de Investigación Severo Ochoa Programme for Centres of Excellence in R&D (CEX2023-001263-S). R.D. thanks the French National Research Agency (STORE-EX Labex Project ANR-10-LABX-76-01) for financial support. M.R. acknowledges the European Union H2020-MSCA-COFUND Program for grant agreement #945357 (DESTINY project). Alistore-European Research Institute is gratefully acknowledged for financial support through the postdoc grant to C.B., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Spin-orbit entanglement driven by the Jahn-Teller effect

Digital.CSIC. Repositorio Institucional del CSIC
  • Miñarro, Alejandro S.
  • Villa, Mario
  • Casals, Blai
  • Plana Ruiz, Sergi
  • Sánchez Barrera, Florencio
  • Gázquez, Jaume
  • Herranz, Gervasi
Spin-orbit entanglement in 4d and 5d transition metal systems can enhance electronic correlations, leading to nontrivial ground states and the emergence of exotic excitations. There is also an interest to investigate spin-orbit entanglement in 3d compounds, though this is challenging due to their smaller spin-orbit coupling. Here we demonstrate that the Jahn-Teller effect in Mn3+ reduces the energy gap between high- and low- spin-orbital states that lead to enhanced spin-orbit entanglement. Our results show a rare example of synergistic effects of Jahn-Teller and spin-orbit interactions and provide a way to entangle different degrees of freedom in d-metal oxides, which may allow paths to explore the interplay of orbital, lattice and spins in 3d correlated systems., We acknowledge financial support from Projects No. PID2023-152225NB-I00, PID2023-147211OB-C21, PID2020-118479RBI00, PID2020-112548RB-I00, and Severo Ochoa MATRANS42 (No. CEX2023-001263-S) of the Spanish Ministry of Science and Innovation (Grant No. MICIU/AEI/10.13039/501100011033 and FEDER, EU)"), Projects No. TED2021-129857B-I00 and TED2021-130453B-C21, funded by MCIN/AEI/10.13039/501100011033 and European Union NextGeneration EU/PRTR and by the Generalitat de Catalunya (2021 SGR 00445, 2021 SGR 00804). We thank the X-ray Diffraction Laboratory at ICMAB-CSIC for their assistance in X-ray diffraction reciprocal space maps. We thank Gyanendra Singh for his participation in formatting some of the figures of the main text. EM02-METCAM at ALBA and ICTS-CNME at UCM are acknowledged for offering access to STEM microscopy and expertise. The authors acknowledge the TEM facilities of the Scientific & Technical Resources Service (SRCiT) from Universitat Rovira i Virgili where the TEM was partially funded by the operative program FEDER Catalunya 2014-2020 (IU16-015844)., info:eu-repo/grantAgreement/AEI/Plan Estatal de investigación Científica y Técnica y de Innovación 2021-2023/CEX2023-001263-S, Peer reviewed




Plasmonic Coupling for High-Sensitivity Detection of Low Molecular Weight Molecules

Digital.CSIC. Repositorio Institucional del CSIC
  • Guglielmelli, Alexa
  • Zaffino, Rossella
  • Palermo, Giovanna
  • Valente, Liliana
  • Aceti, Dante Maria
  • Ricciardi, Loredana
  • González Campo, Arántzazu
  • Pfattner, Raphael
  • Aliaga Alcalde, Núria
  • Strangi, Giuseppe
This article presents a novel plasmonic sensing platform designed for the detection of low molecular weight molecules, offering significant advancements in diagnostic applications. The platform features a periodic array of gold nanodisks on a 20 nm thin silica layer, supported by a 100 nm thick gold substrate. By leveraging the coupling between localized and propagating surface plasmon resonances, this design significantly enhances the sensitivity and specificity of molecular detection. Finite element method simulations are conducted to characterize the optical properties and reflectance response of the nanodisks array in the visible to near-infrared range. Ellipsometric analysis is performed to measure the reflectance of the sample at various angles. Additionally, scanning near-field optical microscopy in reflectance mode validates the design by revealing well-defined plasmonic hot spots and interference patterns consistent with the simulated results. The findings demonstrate the platform's effectiveness in amplifying optical signals, achieving a limit of detection of 50 μM for molecules with a molecular weight of less than 1 KDa. This high sensitivity and specificity highlight the potential of the proposed plasmonic platform to advance the development of highly sensitive sensors for low molecular weight molecules, making it a valuable tool for diagnostics and precise molecular detection., The authors are grateful to Dr. Giovanni Desiderio for SEM measurements and analysis. A.G. acknowledges financial support from the “NLHT- Nanoscience Laboratory for Human Technologies” - (POR Calabria FESR-FSE 14/20 – CUP: J22C14000230007) and POS RADIOAMICA project funded by the Italian Minister of Health (CUP: H53C22000650006). D.M.A. acknowledges financial support from the project progetto PRIN - 2022P9F79R, (CUP: H53D23000830006). This work was also supported by the projects PID2019-108794GBI00 funded by MCIN/AEI/10.13039/501100011033 from the Ministerio de Ciencia e Innovación. The CSIC authors acknowledge the financial support from the Spanish Ministry Science, through the ‘‘Severo Ochoa’’ Programme for Centres of Excellence (MATRANS42, CEX2023-001263-S)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Fluorescent molecular systems based on carborane-perylenediimide conjugates

Digital.CSIC. Repositorio Institucional del CSIC
  • Rodríguez Madrid, Rubén
  • Sinha, Sohini
  • Parejo, Laura
  • Hernando, Jordi
  • Núñez Aguilera, Rosario
This study presents the successful synthesis of two perylenediimide (PDI)-based ortho-carborane (o-carborane) derivatives, PDI-CB1 and PDI-CB2, through the insertion of decaborane into alkyne-terminated PDIs (PDI1 and PDI2). The introduction of o-carborane groups did not alter the optical properties of the PDI units in solution compared to their carborane-free counterparts, maintaining excellent fluorescence quantum yields of around 100% in various solvents. This was achieved by using a methylene linker to minimize electronic interaction between PDI and o-carborane, and by incorporating bulky o-carborane groups at imide- position to enhance solubility and prevent π-π stacking-induced aggregation. Aggregation studies demonstrated that PDI-CB1 and PDI-CB2 have greater solubility than PDI1 and PDI2 in both nonpolar and aqueous solvents. Despite the steric hindrance imparted by the o-carborane units, the solid state emission of PDI-CB1 and PDI-CB2 was affected by aggregation-caused fluorescence quenching. However, solid PDI-CB1 preserved bright red excimer-type emission, which persisted in water-dispersible nanoparticles, indicating potential for application as a theranostic agent combining fluorescence bioimaging with anticancer boron neutron capture therapy (BNCT) due to its high boron content., This work was supported by grants PID2022-141293OB-I00 and PID2022-136892NB-I00 funded by MICIU/AEI/10.13039/501100011033 and by ERDF – “A way of making Europe”. R. Núñez acknowledges financial support from the State Investigation Agency, through the Severo Ochoa Programme for Centers of Excellence in R&D (CEX2023-001263-S). Financial support from the Generalitat de Catalunya (AGAUR) is also acknowledged through 2021 SGR 00064 and 2021 SGR 00442 projects. S. S. acknowledges financial support from DOC-FAM, the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no 754397. L. P. thanks to the Universitat Autònoma de Barcelona for her predoctoral fellowship. J. H. is a Serra Húnter Fellow., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




A new plant-based drug delivery platform based on alkyl polyglucosides and β-sitosterol nanovesicles for topical delivery

Digital.CSIC. Repositorio Institucional del CSIC
  • Alcaina Hernando, Marta
  • Malvacio, Ivana
  • Ferraboschi, Ilaria
  • Huck-Iriart, Cristián
  • Bianchera, Annalisa
  • Sala Vergés, Santiago
  • Pedersen, Jan Skov
  • Ferrer Tasies, Lidia P.
  • Pescina, Silvia
  • Sissa, Cristina
  • Ventosa, Nora
  • Córdoba, Alba
The finding of new vesicular systems is a challenging process that depends on different factors such as the components used, the interactions between them or the dispersant media. Our objective was to develop a new vesicular delivery system formed by self-assembly of β-Sitosterol (Sit), Lauryl Glucoside (LGL) and Lauryl Glucose Carboxylate (LGC) molecules, all plant-based, biodegradable and biocompatible components. Nanovesicles (NVs) with different molar ratios of Sit, LGL and LGC were prepared using a single step method named DELOS, and characterized by dynamic light scattering, cryo-electron microscopy and small-angle X-ray scattering. Antioxidant compound α-tocopherol (TCP) was integrated in the NVs showing their potential to nanoformulate hydrophobic payloads. Finally, in vitro biocompatibility assays with reconstructed human epidermis and ex vivo skin retention studies using multiphoton microscopy and NVs labelled with Nile Red (NR) were carried out. As a result of this work, a new platform of NVs has been obtained by the self-assembly of Sit, LGL and LGC, obtaining vesicular systems with tunable physicochemical properties in terms of size (130 – 220 nm), surface charge ((-70) – (-40) mV) and lamellarity (unilamellar and multilamellar vesicles), when the carbon chain of the alkyl polyglucoside was >12. The vesicles could efficiently integrate TCP, proving their potential role as delivery systems and maintaining its antioxidant activity after loading. Finally, they also showed biocompatibility with the skin and improved the permeability of the poorly water-soluble molecule NR in terms of time and depth through the epidermis. Overall, the results of this work point to the successful development of an attractive platform based on stable and homogeneous nanovesicles composed of plant-derived ingredients for topical delivery., This work was supported by grants of Industrial Doctorates Plan of Ministerio de Ciencia e Innovación (DIN2019–010396) and Industrial Doctorates Plan of Agaur-Generalitat de Catalunya (2020 DI 14). The research leading to these results has also received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 712949 (TECNIOspring PLUS) and from the Agency for Business Competitiveness of the Government of Catalonia. This project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska–Curie grant agreement number 101007804 (Multifunctional nanocarriers for nonlinear microscopy: new tools for biology and medicine (Micro4Nano)). This project has received funding from the European Union´s Horizon 2020 research and innovation programme under grant agreement no. 101004728 via the TamaTA-INNOV call for access to the BL11-NCD-SWEET beamline from the ALBA synchrotron. The work has also been supported by the Spanish Ministry of Science and Innovation through grants "MOL4BIO" (PID2019–105622RB-I00), "ARMONIA" (PID2022–137332OB-I00) and the FUNFUTURE-FIP-2020 Severo Ochoa project, and by the Generalitat de Catalunya through grant 2021 SGR 00438. I. F. benefited of a PhD fellowship financed by PON R&I 2014–2020 (FSE REACT EU fundings). I.F. and C.S. also benefited from the equipment and framework of the COMP-HUB and COMP-R Initiative, funded by the “Departments of Excellence” program of the Italian Ministry for Education, University and Research (MIUR, 2018–2022 and MUR, 2023–2027). NV acknowledges financial support from the State Investigation Agency, through the Severo Ochoa Programme for Centres of Excellence in R&D (CEX2023–001263-S)., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Interface Engineering in All-Oxide Photovoltaic Devices Based on Photoferroelectric BiFe0.9Co0.1O3 Thin Films

Digital.CSIC. Repositorio Institucional del CSIC
  • Machado, Pamela
  • Salles, Pol
  • Frebel, Alexander
  • Luca, Gabriele de
  • Ros, Eloi
  • Hagendorf, Christian
  • Fina, Ignasi
  • Puigdollers, Joaquim
  • Coll, Mariona
Photoferroelectric BiFeO3 (BFO) has attracted renewed interest to be integrated into thin film photovoltaic (PV) devices as a stable, lead-free, and versatile photoabsorber with simplified architecture. While significant efforts have been dedicated toward the exploration of strategies to tailor the properties of this photoabsorber to improve the device performance, efficiencies still remain low. The modification of the BFO interface by the incorporation of transport-selective layers can offer fresh opportunities to modify the properties of the device. Identifying an optical and electrically suitable selective layer while ensuring easy device processing and controlled film properties is challenging. In this work, we determine the influence of incorporating a ZnO layer on the ferroelectric and photoresponse behavior of an epitaxial BiFe0.9Co0.1O3 (BFCO)-based heterostructure. The device is completed with Sn-doped In2O3 (ITO) and La0.7Sr0.3MnO3 (LSMO) electrodes. This all-oxide system is stable under ambient conditions and displays robust ferroelectricity. The coupled ferroelectricity-photoresponse measurements demonstrate that the short circuit current can be modulated by ferroelectric polarization in up to 68% under blue monochromatic light. Also, the responsivity of the system with the ZnO-modified interface is larger than that of the system with no ZnO. Complementary band energy alignment studies reveal that the observed increase in the short circuit current density of the device with ZnO is attributed to lower Fermi level energy at the ZnO/BFCO interface compared to the ITO/BFCO interface, which reduces charge recombination. Therefore, this study provides useful insights into the role of the ZnO interface layer in stable BFO-based devices to further explore their viability for potential optoelectronic applications., This work was funded by CEX2023-001263-S/AEI/10.13039/501100011033, PID2020-535 114224RB-I00/AEI/10.13039/501100011033, PID2019-536 107727RB-I00/AEI/10.13039/501100011033. The authors also acknowledge projects TED2021-130402B-I00 and TED2021-130453B-C21 funded by MICIU/AEI/10.13039/501100011033 and European Union NextGenerationEU/PRTR. The authors acknowledge Prof. Josep Fontcuberta for fruitful scientific discussions on the photoferroelectric behavior of BFCO heterostructures and Prof. Andreas Klein for his advice on XPS data acquisition and energy band alignment interpretation. Dr. G. Sauthier is also acknowledged for the support in the XPS measurements. P.M. and P.S. acknowledge financial support from the FPI fellowship (PRE2018-084618) and from the “la Caixa” Foundation LCF/BQ/DI19/11730026 fellowship. The work of P.M. and P.S. has been done in the framework of the doctorate in Materials Science of the Autonomous University of Barcelona. G.D.L. acknowledges funding from the Swiss National Science Foundation (SNSF) under Project No. P2EZP2-191865 and grant RYC2021-032524-I funded by MCIN/AEI/10.13039/501100011033 and by “European Union NextGenerationEU”/PRTR. G.D.L also acknowledges Prof. G. Catalan for the use of the off-axis sputtering system., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed




Water-Soluble Bimodal Magnetic-Fluorescent Radical Dendrimers as Potential MRI-FI Imaging Probes

Digital.CSIC. Repositorio Institucional del CSIC
  • Wu, Yufei
  • Lloveras, Vega
  • Morgado, Anjara
  • Pérez Inestrosa, Ezequiel
  • Babaliari, Eleftheria
  • Psilodimitrakopoulos, Sotiris
  • Vida, Yolanda
  • Vidal Gancedo, José
Dual or multimodal imaging probes have become potent tools for enhancing detection sensitivity and accuracy in disease diagnosis. In this context, we present a bimodal imaging dendrimer-based structure that integrates magnetic and fluorescent imaging probes for potential applications in magnetic resonance imaging and fluorescence imaging. It stands out as one of the rare examples where bimodal imaging probes use organic radicals as the magnetic source, despite their tendency to entirely quench fluorophore fluorescence. Opting for organic radicals over metal-based contrast agents like gadolinium (Gd3+)-chelates is crucial to mitigate associated toxicity concerns. We utilized an amino-terminated polyamide dendrimer containing a 1,8-naphthalimide (Naft) fluorescent group, amino acid derivatives as linkers to enhance water solubility, and TEMPO organic radicals as terminal groups. The same dendrimer structure, featuring an equivalent number of branches but lacking the fluorophore group, was also functionalized with amino acid and terminal radicals to serve as a reference. Remarkably, we achieved a fully water-soluble dendrimer-based structure exhibiting both magnetic and fluorescent properties simultaneously. The fluorescence of the Naft group in the final structure is somewhat quenched by the organic radicals, likely due to photoinduced electron transfer with the nitroxyl radical acting as an electron acceptor, which has been supported by density functional theory calculations. Molecular dynamics simulations are employed to investigate how the dendrimers' structure influences the electron paramagnetic resonance characteristics, relaxivity, and fluorescence. In summary, despite the influence of the radicals-fluorophore interactions on fluorescence, this bimodal dendrimer demonstrates significant fluorescent properties and effective r1 relaxivity of 1.3 mM-1 s-1. These properties have proven effective in staining the live mesenchymal stem cells without affecting the cell nucleus., This work was funded by Ministerio de Ciencia, Innovación y
Universidades MICIU (PID2022-137332OB-I00, PID2022-
136705NB-I00 and Severo Ochoa FUNFUTURE-FIP-2020
Viraden FYP-3 projects), Generalitat de Catalunya (2021 SGR
00438), CIBER-BBN (BBN23PIV01 project) and Intramural
CSIC project 202360E61. ICMAB acknowledges Spanish
MICIU/AEI through the Severo Ochoa Centres of Excellence
Programme Grant CEX2019-000917-S and CEX2023-001263-
S. This work was supported by the NFFA EUROPE Pilot (EU
2020 framework programme) under grant agreement
no.101007417 from 1/03/2021 to 28/02/2026 within the
framework of the NFFA-Europe Staff Exchanges for Access
Providers. We thank Dr. Silvia Lope of the NMR service of
Universitat Autonoma ̀ de Barcelona (UAB) for the MRI
phantoms measurements and Prof. Gunnar Jeschke for his
valuable comments and help on the EPR simulation. Y.W.
acknowledges his China Scholarship Council (CSC) grant., With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).
With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2023-001263-S)., Peer reviewed