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Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors

[Image: see text] Halide perovskites are versatile semiconductors with applications including photovoltaics and light-emitting devices, having modular optoelectronic properties realizable through composition and dimensionality tuning. Layered Ruddlesden–Popper perovskites are particularly interestin...

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Autores principales: Baldwin, Alan, Delport, Géraud, Leng, Kai, Chahbazian, Rosemonde, Galkowski, Krzysztof, Loh, Kian Ping, Stranks, Samuel D.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8154849/
https://www.ncbi.nlm.nih.gov/pubmed/33877840
http://dx.doi.org/10.1021/acs.jpclett.1c00823
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author Baldwin, Alan
Delport, Géraud
Leng, Kai
Chahbazian, Rosemonde
Galkowski, Krzysztof
Loh, Kian Ping
Stranks, Samuel D.
author_facet Baldwin, Alan
Delport, Géraud
Leng, Kai
Chahbazian, Rosemonde
Galkowski, Krzysztof
Loh, Kian Ping
Stranks, Samuel D.
author_sort Baldwin, Alan
collection PubMed
description [Image: see text] Halide perovskites are versatile semiconductors with applications including photovoltaics and light-emitting devices, having modular optoelectronic properties realizable through composition and dimensionality tuning. Layered Ruddlesden–Popper perovskites are particularly interesting due to their unique 2D character and charge carrier dynamics. However, long-range energy transport through exciton diffusion in these materials is not understood or realized. Here, local time-resolved luminescence mapping techniques are employed to visualize exciton transport in exfoliated flakes of the BA(2)MA(n–1)Pb(n)I(3n+1) perovskite family. Two distinct transport regimes are uncovered, depending on the temperature range. Above 100 K, diffusion is mediated by thermally activated hopping processes between localized states. At lower temperatures, a nonuniform energy landscape emerges in which transport is dominated by downhill energy transfer to lower-energy states, leading to long-range transport over hundreds of nanometers. Efficient, long-range, and switchable downhill transfer offers exciting possibilities for controlled directional long-range transport in these 2D materials for new applications.
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spelling pubmed-81548492021-05-27 Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors Baldwin, Alan Delport, Géraud Leng, Kai Chahbazian, Rosemonde Galkowski, Krzysztof Loh, Kian Ping Stranks, Samuel D. J Phys Chem Lett [Image: see text] Halide perovskites are versatile semiconductors with applications including photovoltaics and light-emitting devices, having modular optoelectronic properties realizable through composition and dimensionality tuning. Layered Ruddlesden–Popper perovskites are particularly interesting due to their unique 2D character and charge carrier dynamics. However, long-range energy transport through exciton diffusion in these materials is not understood or realized. Here, local time-resolved luminescence mapping techniques are employed to visualize exciton transport in exfoliated flakes of the BA(2)MA(n–1)Pb(n)I(3n+1) perovskite family. Two distinct transport regimes are uncovered, depending on the temperature range. Above 100 K, diffusion is mediated by thermally activated hopping processes between localized states. At lower temperatures, a nonuniform energy landscape emerges in which transport is dominated by downhill energy transfer to lower-energy states, leading to long-range transport over hundreds of nanometers. Efficient, long-range, and switchable downhill transfer offers exciting possibilities for controlled directional long-range transport in these 2D materials for new applications. American Chemical Society 2021-04-20 2021-04-29 /pmc/articles/PMC8154849/ /pubmed/33877840 http://dx.doi.org/10.1021/acs.jpclett.1c00823 Text en © 2021 The Authors. Published by American Chemical Society Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Baldwin, Alan
Delport, Géraud
Leng, Kai
Chahbazian, Rosemonde
Galkowski, Krzysztof
Loh, Kian Ping
Stranks, Samuel D.
Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors
title Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors
title_full Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors
title_fullStr Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors
title_full_unstemmed Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors
title_short Local Energy Landscape Drives Long-Range Exciton Diffusion in Two-Dimensional Halide Perovskite Semiconductors
title_sort local energy landscape drives long-range exciton diffusion in two-dimensional halide perovskite semiconductors
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8154849/
https://www.ncbi.nlm.nih.gov/pubmed/33877840
http://dx.doi.org/10.1021/acs.jpclett.1c00823
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