Multi-cation perovskites prevent carrier reflection from grain surfaces

© 2020, The Author(s), under exclusive licence to Springer Nature Limited. The composition of perovskite has been optimized combinatorially such that it often contains six components (AxByC1−x−yPbXzY3−z) in state-of-art perovskite solar cells. Questions remain regarding the precise role of each comp...

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Main Authors: Saidaminov, Makhsud I, Williams, Kristopher, Wei, Mingyang, Johnston, Andrew, Quintero-Bermudez, Rafael, Vafaie, Maral, Pina, Joao M, Proppe, Andrew H, Hou, Yi, Walters, Grant, Kelley, Shana O, Tisdale, William A, Sargent, Edward H
Format: Article
Language:English
Published: Springer Science and Business Media LLC 2021
Online Access:https://hdl.handle.net/1721.1/136573
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author Saidaminov, Makhsud I
Williams, Kristopher
Wei, Mingyang
Johnston, Andrew
Quintero-Bermudez, Rafael
Vafaie, Maral
Pina, Joao M
Proppe, Andrew H
Hou, Yi
Walters, Grant
Kelley, Shana O
Tisdale, William A
Sargent, Edward H
author_facet Saidaminov, Makhsud I
Williams, Kristopher
Wei, Mingyang
Johnston, Andrew
Quintero-Bermudez, Rafael
Vafaie, Maral
Pina, Joao M
Proppe, Andrew H
Hou, Yi
Walters, Grant
Kelley, Shana O
Tisdale, William A
Sargent, Edward H
author_sort Saidaminov, Makhsud I
collection MIT
description © 2020, The Author(s), under exclusive licence to Springer Nature Limited. The composition of perovskite has been optimized combinatorially such that it often contains six components (AxByC1−x−yPbXzY3−z) in state-of-art perovskite solar cells. Questions remain regarding the precise role of each component, and the lack of a mechanistic explanation limits the practical exploration of the large and growing chemical space. Here, aided by transient photoluminescence microscopy, we find that, in perovskite single crystals, carrier diffusivity is in fact independent of composition. In polycrystalline thin films, the different compositions play a crucial role in carrier diffusion. We report that methylammonium (MA)-based films show a high carrier diffusivity of 0.047 cm2 s−1, while MA-free mixed caesium-formamidinium (CsFA) films exhibit an order of magnitude lower diffusivity. Elemental composition studies show that CsFA grains display a graded composition. This curtails electron diffusion in these films, as seen in both vertical carrier transport and surface potential studies. Incorporation of MA leads to a uniform grain core-to-edge composition, giving rise to a diffusivity of 0.034 cm2 s−1 in CsMAFA films. A model that invokes competing crystallization processes allows us to account for this finding, and suggests further strategies to achieve homogeneous crystallization for the benefit of perovskite optoelectronics.
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spelling mit-1721.1/1365732021-10-28T03:10:29Z Multi-cation perovskites prevent carrier reflection from grain surfaces Saidaminov, Makhsud I Williams, Kristopher Wei, Mingyang Johnston, Andrew Quintero-Bermudez, Rafael Vafaie, Maral Pina, Joao M Proppe, Andrew H Hou, Yi Walters, Grant Kelley, Shana O Tisdale, William A Sargent, Edward H © 2020, The Author(s), under exclusive licence to Springer Nature Limited. The composition of perovskite has been optimized combinatorially such that it often contains six components (AxByC1−x−yPbXzY3−z) in state-of-art perovskite solar cells. Questions remain regarding the precise role of each component, and the lack of a mechanistic explanation limits the practical exploration of the large and growing chemical space. Here, aided by transient photoluminescence microscopy, we find that, in perovskite single crystals, carrier diffusivity is in fact independent of composition. In polycrystalline thin films, the different compositions play a crucial role in carrier diffusion. We report that methylammonium (MA)-based films show a high carrier diffusivity of 0.047 cm2 s−1, while MA-free mixed caesium-formamidinium (CsFA) films exhibit an order of magnitude lower diffusivity. Elemental composition studies show that CsFA grains display a graded composition. This curtails electron diffusion in these films, as seen in both vertical carrier transport and surface potential studies. Incorporation of MA leads to a uniform grain core-to-edge composition, giving rise to a diffusivity of 0.034 cm2 s−1 in CsMAFA films. A model that invokes competing crystallization processes allows us to account for this finding, and suggests further strategies to achieve homogeneous crystallization for the benefit of perovskite optoelectronics. 2021-10-27T20:36:03Z 2021-10-27T20:36:03Z 2020 2021-06-15T14:18:18Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/136573 en 10.1038/S41563-019-0602-2 Nature Materials Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf Springer Science and Business Media LLC other univ website
spellingShingle Saidaminov, Makhsud I
Williams, Kristopher
Wei, Mingyang
Johnston, Andrew
Quintero-Bermudez, Rafael
Vafaie, Maral
Pina, Joao M
Proppe, Andrew H
Hou, Yi
Walters, Grant
Kelley, Shana O
Tisdale, William A
Sargent, Edward H
Multi-cation perovskites prevent carrier reflection from grain surfaces
title Multi-cation perovskites prevent carrier reflection from grain surfaces
title_full Multi-cation perovskites prevent carrier reflection from grain surfaces
title_fullStr Multi-cation perovskites prevent carrier reflection from grain surfaces
title_full_unstemmed Multi-cation perovskites prevent carrier reflection from grain surfaces
title_short Multi-cation perovskites prevent carrier reflection from grain surfaces
title_sort multi cation perovskites prevent carrier reflection from grain surfaces
url https://hdl.handle.net/1721.1/136573
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