Dataset.

Effect of Connectivity on the Carrier Transport and Recombination Dynamics of Perovskite Quantum-Dot Networks [Dataset]

Digital.CSIC. Repositorio Institucional del CSIC
oai:digital.csic.es:10261/359752
Digital.CSIC. Repositorio Institucional del CSIC
  • Tiede, David O.
  • Romero-Pérez, Carlos
  • Koch, Katherine A.
  • Ucer, K. Burak
  • Calvo, Mauricio E.
  • Srimath Kandada, Ajay Ram
  • Galisteo-López, Juan F.
  • Míguez, Hernán
Quantum-dot (QD) solids are being widely exploited as a solution-processable technology to develop photovoltaic, light-emission, and photodetection devices. Charge transport in these materials is the result of a compromise between confinement at the individual QD level and electronic coupling among the different nanocrystals in the ensemble. While this is commonly achieved by ligand engineering in colloidal-based systems, ligand-free QD assemblies have recently emerged as an exciting alternative where nanostructures can be directly grown into porous matrices with optical quality as well as control over their connectivity and, hence, charge transport properties. In this context, we present a complete photophysical study comprising fluence- and temperature-dependent timeresolved spectroscopy to study carrier dynamics in ligand-free QD networks with gradually varying degrees of interconnectivity, which we achieve by changing the average distance between the QDs. Analysis of the photoluminescence and absorption properties of the QD assemblies, involving both static and timeresolved measurements, allows us to identify the weight of the different recombination mechanisms, both radiative and nonradiative, as a function of QD connectivity. We propose a picture where carrier diffusion, which is needed for any optoelectronic application and implies interparticle transport, gives rise to the exposure of carriers to a larger defect landscape than in the case of isolated QDs. The use of a broad range of fluences permits extracting valuable information for applications demanding either low- or high-carrier-injection levels and highlighting the relevance of a judicious design to balance recombination and diffusion., HM is thankful for the financial support of the Spanish Ministry of Science and Innovation under grant PID2020-116593RB-I00, funded by MCIN/AEI/10.13039/501100011033, and of the Junta de Andalucía under grant P18-RT-2291 (FEDER/UE). HM, JFGL, and DOT acknowledge financial support from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 956270 (Persephone). ARSK acknowledges the start-up funds provided by Wake Forest University and funding from the Center for Functional Materials and the Office of Research and Sponsored Programs at WFU., (Folder > File.txt) Figure 1 Figure_1c(norm. Abs).txt Figure_1d(PL).txt Figure_1e(PLQY).txt Figure 2 Figure_2a (TRPL_raw_bulk).txt Figure_2b (TRPL_raw_30per).txt Figure_2c (TRPL_raw_20per).txt Figure_2d (TRPL_raw_10per).txt Figure_2e (TRPL_raw_5per).txt Figure_2i (TRPL_photon_flux_bulk).txt Figure_2j (TRPL_photon_flux_30per).txt Figure_2k (TRPL_photon_flux_20per).txt Figure_2l (TRPL_photon_flux_10per).txt Figure_2m (TRPL_photon_flux_5per).txt Figure 3 Figure_3a (PLQY_bulk).txt Figure_3b (rel_PLQY_Tdep_30per).txt Figure_3c (rel_PLQY_Tdep_20per).txt Figure_3d (rel_PLQY_Tdep_10per).txt Figure_3e (rel_PLQY_Tdep_5per).txt Figure 4 Figure_4a (30per_norm_PL_80K).txt Figure_4b (5per_norm_PL_80K).txt Figure_4c (30per_TA_77K_N=15d5).csv Figure_4d (5per_TA_77K_N=11d1).csv Figure 5 Figure 5a (30per_GSB_decay).txt Figure 5b (5per_GSB_decay).txt Figure 5c (30per_GSB_decay_derivative).txt Figure 5d (5per_GSB_decay_biexciton_fit_all).txt, Peer reviewed
 

DOI: http://hdl.handle.net/10261/359752, https://doi.org/10.20350/digitalCSIC/16343
Digital.CSIC. Repositorio Institucional del CSIC
oai:digital.csic.es:10261/359752

HANDLE: http://hdl.handle.net/10261/359752, https://doi.org/10.20350/digitalCSIC/16343
Digital.CSIC. Repositorio Institucional del CSIC
oai:digital.csic.es:10261/359752
 
Ver en: http://hdl.handle.net/10261/359752, https://doi.org/10.20350/digitalCSIC/16343
Digital.CSIC. Repositorio Institucional del CSIC
oai:digital.csic.es:10261/359752

Digital.CSIC. Repositorio Institucional del CSIC
oai:digital.csic.es:10261/350930
Artículo científico (article). 2024

EFFECT OF CONNECTIVITY ON THE CARRIER TRANSPORT AND RECOMBINATION DYNAMICS OF PEROVSKITE QUANTUM-DOT NETWORKS

Digital.CSIC. Repositorio Institucional del CSIC
  • Tiede, David O.
  • Romero-Pérez, Carlos
  • Koch, Katherine A.
  • Ucer, K. Burak
  • Calvo, Mauricio E.
  • Srimath Kandada, Ajay Ram
  • Galisteo-López, Juan F.
  • Míguez, Hernán
Quantum-dot (QD) solids are being widely exploited as a solution-processable technology to develop photovoltaic, light-emission, and photodetection devices. Charge transport in these materials is the result of a compromise between confinement at the individual QD level and electronic coupling among the different nanocrystals in the ensemble. While this is commonly achieved by ligand engineering in colloidal-based systems, ligand-free QD assemblies have recently emerged as an exciting alternative where nanostructures can be directly grown into porous matrices with optical quality as well as control over their connectivity and, hence, charge transport properties. In this context, we present a complete photophysical study comprising fluence- and temperature-dependent time-resolved spectroscopy to study carrier dynamics in ligand-free QD networks with gradually varying degrees of interconnectivity, which we achieve by changing the average distance between the QDs. Analysis of the photoluminescence and absorption properties of the QD assemblies, involving both static and time-resolved measurements, allows us to identify the weight of the different recombination mechanisms, both radiative and nonradiative, as a function of QD connectivity. We propose a picture where carrier diffusion, which is needed for any optoelectronic application and implies interparticle transport, gives rise to the exposure of carriers to a larger defect landscape than in the case of isolated QDs. The use of a broad range of fluences permits extracting valuable information for applications demanding either low- or high-carrier-injection levels and highlighting the relevance of a judicious design to balance recombination and diffusion., HM is thankful for the financial support of the Spanish Ministry of Science and Innovation under grant PID2020- 116593RB-I00, funded by MCIN/AEI/10.13039/501100011033, and of the Junta de Andalucía under grant P18-RT-2291 (FEDER/UE). HM, JFGL, and DOT acknowledge financial support from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 956270 (Persephone). ARSK acknowledges the start-up funds provided by Wake Forest University and funding from the Center for Functional Materials and, Peer reviewed




Digital.CSIC. Repositorio Institucional del CSIC
oai:digital.csic.es:10261/352717
Artículo científico antes de ser publicado, versión del autor (preprint). 2023

EFFECT OF CONNECTIVITY ON THE CARRIER TRANSPORT AND RECOMBINATION DYNAMICS OF PEROVSKITE QUANTUM DOT NETWORKS

Digital.CSIC. Repositorio Institucional del CSIC
  • Tiede, David O.
  • Romero-Pérez, Carlos
  • Koch, Katherine A.
  • Ucer, K. Burak
  • Calvo, Mauricio E.
  • Srimath Kandada, Ajay Ram
  • Galisteo-López, Juan F.
  • Míguez, Hernán
Quantum dot (QD) solids are being widely exploited as a solution-processable technology to develop photovoltaic, light-emission, and photo-detection devices. Charge transport in these materials is the result of a compromise between confinement at the individual QD level and electronic coupling among the different nanocrystals in the ensemble. While this is commonly achieved by ligand engineering in colloidal-based systems, ligand-free QD assemblies have recently emerged as an exciting alternative where nanostructures can be directly grown into porous matrices with optical quality as well as control over their connectivity and hence charge transport properties. In this context, we present a complete photophysical study comprising fluence and temperature-dependent time-resolved spectroscopy to study carrier dynamics in ligand-free QD networks with gradually varying degrees of interconnectivity, which we achieve by changing the average distance between the QDs. Analysis of the photoluminescence and absorption properties of the QD assemblies, involving both static and time-resolved measurements, allows us to identify the weight of the different recombination mechanisms, both radiative and non-radiative, as a function of QD connectivity. We propose a picture where carrier diffusion, which is needed for any optoelectronic application and implies inter-particle transport, gives rise to the exposure of carriers to a larger defect landscape than in the case of isolated QDs. The use of a broad range of fluences permits extracting valuable information for applications demanding either low or high carrier injection levels and highlighting the relevance of a judicious design to balance recombination and diffusion., HM is thankful for the financial support of the Spanish Ministry of Science and Innovation under grant PID2020-116593RB-I00, funded by MCIN/AEI/10.13039/501100011033, and of the Junta de Andalucía under grant P18-RT-2291 (FEDER/UE). HM, JFGL, and DOT acknowledge financial support from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 956270 (Persephone). ARSK acknowledges the start-up funds provided by Wake Forest University and funding from the Center for Functional Materials and the Office of Research and Sponsored Programs at WFU., No




Digital.CSIC. Repositorio Institucional del CSIC
oai:digital.csic.es:10261/359752
Dataset. 2024

EFFECT OF CONNECTIVITY ON THE CARRIER TRANSPORT AND RECOMBINATION DYNAMICS OF PEROVSKITE QUANTUM-DOT NETWORKS [DATASET]

Digital.CSIC. Repositorio Institucional del CSIC
  • Tiede, David O.
  • Romero-Pérez, Carlos
  • Koch, Katherine A.
  • Ucer, K. Burak
  • Calvo, Mauricio E.
  • Srimath Kandada, Ajay Ram
  • Galisteo-López, Juan F.
  • Míguez, Hernán
Quantum-dot (QD) solids are being widely exploited as a solution-processable technology to develop photovoltaic, light-emission, and photodetection devices. Charge transport in these materials is the result of a compromise between confinement at the individual QD level and electronic coupling among the different nanocrystals in the ensemble. While this is commonly achieved by ligand engineering in colloidal-based systems, ligand-free QD assemblies have recently emerged as an exciting alternative where nanostructures can be directly grown into porous matrices with optical quality as well as control over their connectivity and, hence, charge transport properties. In this context, we present a complete photophysical study comprising fluence- and temperature-dependent timeresolved spectroscopy to study carrier dynamics in ligand-free QD networks with gradually varying degrees of interconnectivity, which we achieve by changing the average distance between the QDs. Analysis of the photoluminescence and absorption properties of the QD assemblies, involving both static and timeresolved measurements, allows us to identify the weight of the different recombination mechanisms, both radiative and nonradiative, as a function of QD connectivity. We propose a picture where carrier diffusion, which is needed for any optoelectronic application and implies interparticle transport, gives rise to the exposure of carriers to a larger defect landscape than in the case of isolated QDs. The use of a broad range of fluences permits extracting valuable information for applications demanding either low- or high-carrier-injection levels and highlighting the relevance of a judicious design to balance recombination and diffusion., HM is thankful for the financial support of the Spanish Ministry of Science and Innovation under grant PID2020-116593RB-I00, funded by MCIN/AEI/10.13039/501100011033, and of the Junta de Andalucía under grant P18-RT-2291 (FEDER/UE). HM, JFGL, and DOT acknowledge financial support from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 956270 (Persephone). ARSK acknowledges the start-up funds provided by Wake Forest University and funding from the Center for Functional Materials and the Office of Research and Sponsored Programs at WFU., (Folder > File.txt) Figure 1 Figure_1c(norm. Abs).txt Figure_1d(PL).txt Figure_1e(PLQY).txt Figure 2 Figure_2a (TRPL_raw_bulk).txt Figure_2b (TRPL_raw_30per).txt Figure_2c (TRPL_raw_20per).txt Figure_2d (TRPL_raw_10per).txt Figure_2e (TRPL_raw_5per).txt Figure_2i (TRPL_photon_flux_bulk).txt Figure_2j (TRPL_photon_flux_30per).txt Figure_2k (TRPL_photon_flux_20per).txt Figure_2l (TRPL_photon_flux_10per).txt Figure_2m (TRPL_photon_flux_5per).txt Figure 3 Figure_3a (PLQY_bulk).txt Figure_3b (rel_PLQY_Tdep_30per).txt Figure_3c (rel_PLQY_Tdep_20per).txt Figure_3d (rel_PLQY_Tdep_10per).txt Figure_3e (rel_PLQY_Tdep_5per).txt Figure 4 Figure_4a (30per_norm_PL_80K).txt Figure_4b (5per_norm_PL_80K).txt Figure_4c (30per_TA_77K_N=15d5).csv Figure_4d (5per_TA_77K_N=11d1).csv Figure 5 Figure 5a (30per_GSB_decay).txt Figure 5b (5per_GSB_decay).txt Figure 5c (30per_GSB_decay_derivative).txt Figure 5d (5per_GSB_decay_biexciton_fit_all).txt, Peer reviewed





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