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Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals

[Image: see text] Metal-halide perovskite nanocrystals have demonstrated excellent optoelectronic properties for light-emitting applications. Isovalent doping with various metals (M(2+)) can be used to tailor and enhance their light emission. Although crucial to maximize performance, an understandin...

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Autores principales: Ahmed, Ghada H., Liu, Yun, Bravić, Ivona, Ng, Xejay, Heckelmann, Ina, Narayanan, Pournima, Fernández, Martin S., Monserrat, Bartomeu, Congreve, Daniel N., Feldmann, Sascha
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9437917/
https://www.ncbi.nlm.nih.gov/pubmed/35977424
http://dx.doi.org/10.1021/jacs.2c07111
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author Ahmed, Ghada H.
Liu, Yun
Bravić, Ivona
Ng, Xejay
Heckelmann, Ina
Narayanan, Pournima
Fernández, Martin S.
Monserrat, Bartomeu
Congreve, Daniel N.
Feldmann, Sascha
author_facet Ahmed, Ghada H.
Liu, Yun
Bravić, Ivona
Ng, Xejay
Heckelmann, Ina
Narayanan, Pournima
Fernández, Martin S.
Monserrat, Bartomeu
Congreve, Daniel N.
Feldmann, Sascha
author_sort Ahmed, Ghada H.
collection PubMed
description [Image: see text] Metal-halide perovskite nanocrystals have demonstrated excellent optoelectronic properties for light-emitting applications. Isovalent doping with various metals (M(2+)) can be used to tailor and enhance their light emission. Although crucial to maximize performance, an understanding of the universal working mechanism for such doping is still missing. Here, we directly compare the optical properties of nanocrystals containing the most commonly employed dopants, fabricated under identical synthesis conditions. We show for the first time unambiguously, and supported by first-principles calculations and molecular orbital theory, that element-unspecific symmetry-breaking rather than element-specific electronic effects dominate these properties under device-relevant conditions. The impact of most dopants on the perovskite electronic structure is predominantly based on local lattice periodicity breaking and resulting charge carrier localization, leading to enhanced radiative recombination, while dopant-specific hybridization effects play a secondary role. Our results suggest specific guidelines for selecting a dopant to maximize the performance of perovskite emitters in the desired optoelectronic devices.
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spelling pubmed-94379172022-09-03 Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals Ahmed, Ghada H. Liu, Yun Bravić, Ivona Ng, Xejay Heckelmann, Ina Narayanan, Pournima Fernández, Martin S. Monserrat, Bartomeu Congreve, Daniel N. Feldmann, Sascha J Am Chem Soc [Image: see text] Metal-halide perovskite nanocrystals have demonstrated excellent optoelectronic properties for light-emitting applications. Isovalent doping with various metals (M(2+)) can be used to tailor and enhance their light emission. Although crucial to maximize performance, an understanding of the universal working mechanism for such doping is still missing. Here, we directly compare the optical properties of nanocrystals containing the most commonly employed dopants, fabricated under identical synthesis conditions. We show for the first time unambiguously, and supported by first-principles calculations and molecular orbital theory, that element-unspecific symmetry-breaking rather than element-specific electronic effects dominate these properties under device-relevant conditions. The impact of most dopants on the perovskite electronic structure is predominantly based on local lattice periodicity breaking and resulting charge carrier localization, leading to enhanced radiative recombination, while dopant-specific hybridization effects play a secondary role. Our results suggest specific guidelines for selecting a dopant to maximize the performance of perovskite emitters in the desired optoelectronic devices. American Chemical Society 2022-08-17 2022-08-31 /pmc/articles/PMC9437917/ /pubmed/35977424 http://dx.doi.org/10.1021/jacs.2c07111 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/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 Ahmed, Ghada H.
Liu, Yun
Bravić, Ivona
Ng, Xejay
Heckelmann, Ina
Narayanan, Pournima
Fernández, Martin S.
Monserrat, Bartomeu
Congreve, Daniel N.
Feldmann, Sascha
Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals
title Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals
title_full Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals
title_fullStr Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals
title_full_unstemmed Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals
title_short Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals
title_sort luminescence enhancement due to symmetry breaking in doped halide perovskite nanocrystals
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9437917/
https://www.ncbi.nlm.nih.gov/pubmed/35977424
http://dx.doi.org/10.1021/jacs.2c07111
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