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Autori principali: Frohna, Kyle, Chosy, Cullen, Al-Ashouri, Amran, Scheler, Florian, Chiang, Yu-Hsien, Dubajic, Milos, Parker, Julia E., Walker, Jessica M., Zimmermann, Lea, Selby, Thomas A., Lu, Yang, Roose, Bart, Albrecht, Steve, Anaya, Miguel, Stranks, Samuel D.
Natura: Preprint
Pubblicazione: 2024
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Accesso online:https://arxiv.org/abs/2403.16988
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author Frohna, Kyle
Chosy, Cullen
Al-Ashouri, Amran
Scheler, Florian
Chiang, Yu-Hsien
Dubajic, Milos
Parker, Julia E.
Walker, Jessica M.
Zimmermann, Lea
Selby, Thomas A.
Lu, Yang
Roose, Bart
Albrecht, Steve
Anaya, Miguel
Stranks, Samuel D.
author_facet Frohna, Kyle
Chosy, Cullen
Al-Ashouri, Amran
Scheler, Florian
Chiang, Yu-Hsien
Dubajic, Milos
Parker, Julia E.
Walker, Jessica M.
Zimmermann, Lea
Selby, Thomas A.
Lu, Yang
Roose, Bart
Albrecht, Steve
Anaya, Miguel
Stranks, Samuel D.
contents Next-generation low-cost semiconductors such as halide perovskites exhibit optoelectronic properties dominated by nanoscale variations in their structure, composition and photophysics. While microscopy provides a proxy for ultimate device function, past works have focused on neat thin-films on insulating substrates, missing crucial information about charge extraction losses and recombination losses introduced by transport layers. Here we use a multimodal operando microscopy toolkit to measure nanoscale current-voltage curves, recombination losses and chemical composition in an array of state-of-the-art perovskite solar cells before and after extended operational stress. We apply this toolkit to the same scan areas before and after extended operation to reveal that devices with the highest performance have the lowest initial performance spatial heterogeneity - a crucial link that is missed in conventional microscopy. We find that subtle compositional engineering of the perovskite has surprising effects on local disorder and resilience to operational stress. Minimising variations in local efficiency, rather than compositional disorder, is predictive of improved performance and stability. Modulating the interfaces with different contact layers or passivation treatments can increase initial performance but can also lead to dramatic nanoscale, interface-dominated degradation even in the presence of local performance homogeneity, inducing spatially varying transport, recombination, and electrical losses. These operando measurements of full devices act as screenable diagnostic tools, uniquely unveiling the microscopic mechanistic origins of device performance losses and degradation in an array of halide perovskite devices and treatments. This information in turn reveals guidelines for future improvements to both performance and stability.
format Preprint
id arxiv_https___arxiv_org_abs_2403_16988
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Multimodal operando microscopy reveals that interfacial chemistry and nanoscale performance disorder dictate perovskite solar cell stability
Frohna, Kyle
Chosy, Cullen
Al-Ashouri, Amran
Scheler, Florian
Chiang, Yu-Hsien
Dubajic, Milos
Parker, Julia E.
Walker, Jessica M.
Zimmermann, Lea
Selby, Thomas A.
Lu, Yang
Roose, Bart
Albrecht, Steve
Anaya, Miguel
Stranks, Samuel D.
Chemical Physics
Optics
Next-generation low-cost semiconductors such as halide perovskites exhibit optoelectronic properties dominated by nanoscale variations in their structure, composition and photophysics. While microscopy provides a proxy for ultimate device function, past works have focused on neat thin-films on insulating substrates, missing crucial information about charge extraction losses and recombination losses introduced by transport layers. Here we use a multimodal operando microscopy toolkit to measure nanoscale current-voltage curves, recombination losses and chemical composition in an array of state-of-the-art perovskite solar cells before and after extended operational stress. We apply this toolkit to the same scan areas before and after extended operation to reveal that devices with the highest performance have the lowest initial performance spatial heterogeneity - a crucial link that is missed in conventional microscopy. We find that subtle compositional engineering of the perovskite has surprising effects on local disorder and resilience to operational stress. Minimising variations in local efficiency, rather than compositional disorder, is predictive of improved performance and stability. Modulating the interfaces with different contact layers or passivation treatments can increase initial performance but can also lead to dramatic nanoscale, interface-dominated degradation even in the presence of local performance homogeneity, inducing spatially varying transport, recombination, and electrical losses. These operando measurements of full devices act as screenable diagnostic tools, uniquely unveiling the microscopic mechanistic origins of device performance losses and degradation in an array of halide perovskite devices and treatments. This information in turn reveals guidelines for future improvements to both performance and stability.
title Multimodal operando microscopy reveals that interfacial chemistry and nanoscale performance disorder dictate perovskite solar cell stability
topic Chemical Physics
Optics
url https://arxiv.org/abs/2403.16988