Polaron self-localization in white-light emitting hybrid perovskites

Two-dimensional (2D) perovskites with the general formula APbX4 are attracting increasing interest as solution processable, white-light emissive materials. Recent studies have shown that their broadband emission is related to the formation of intra-gap colour centres. Here, we provide an in-depth de...

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Main Authors: Cortecchia, Daniele, Yin, Jun, Bruno, Annalisa, Lo, Shu-Zee Alencious, Gurzadyan, Gagik G., Mhaisalkar, Subodh, Brédas, Jean-Luc, Soci, Cesare
Other Authors: Interdisciplinary Graduate School (IGS)
Format: Journal Article
Language:English
Published: 2017
Subjects:
Online Access:https://hdl.handle.net/10356/82288
http://hdl.handle.net/10220/43518
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author Cortecchia, Daniele
Yin, Jun
Bruno, Annalisa
Lo, Shu-Zee Alencious
Gurzadyan, Gagik G.
Mhaisalkar, Subodh
Brédas, Jean-Luc
Soci, Cesare
author2 Interdisciplinary Graduate School (IGS)
author_facet Interdisciplinary Graduate School (IGS)
Cortecchia, Daniele
Yin, Jun
Bruno, Annalisa
Lo, Shu-Zee Alencious
Gurzadyan, Gagik G.
Mhaisalkar, Subodh
Brédas, Jean-Luc
Soci, Cesare
author_sort Cortecchia, Daniele
collection NTU
description Two-dimensional (2D) perovskites with the general formula APbX4 are attracting increasing interest as solution processable, white-light emissive materials. Recent studies have shown that their broadband emission is related to the formation of intra-gap colour centres. Here, we provide an in-depth description of the charge localization sites underlying the generation of such radiative centres and their corresponding decay dynamics, highlighting the formation of small polarons trapped within their lattice distortion field. Using a combination of spectroscopic techniques and first-principles calculations to study the white-light emitting 2D perovskites (EDBE)PbCl4 and (EDBE)PbBr4, we infer the formation of Pb23+, Pb3+, and X2- (where X = Cl or Br) species confined within the inorganic perovskite framework. Due to strong Coulombic interactions, these species retain their original excitonic character and form self-trapped polaron–excitons acting as radiative colour centres. These findings are expected to be relevant for a broad class of white-light emitting perovskites with large polaron relaxation energy.
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spelling ntu-10356/822882021-01-14T06:25:04Z Polaron self-localization in white-light emitting hybrid perovskites Cortecchia, Daniele Yin, Jun Bruno, Annalisa Lo, Shu-Zee Alencious Gurzadyan, Gagik G. Mhaisalkar, Subodh Brédas, Jean-Luc Soci, Cesare Interdisciplinary Graduate School (IGS) School of Physical and Mathematical Sciences Centre for Disruptive Photonic Technologies (CDPT) Energy Research Institute @ NTU (ERI@N) Two-dimensional perovskites White-light emitting perovskites Two-dimensional (2D) perovskites with the general formula APbX4 are attracting increasing interest as solution processable, white-light emissive materials. Recent studies have shown that their broadband emission is related to the formation of intra-gap colour centres. Here, we provide an in-depth description of the charge localization sites underlying the generation of such radiative centres and their corresponding decay dynamics, highlighting the formation of small polarons trapped within their lattice distortion field. Using a combination of spectroscopic techniques and first-principles calculations to study the white-light emitting 2D perovskites (EDBE)PbCl4 and (EDBE)PbBr4, we infer the formation of Pb23+, Pb3+, and X2- (where X = Cl or Br) species confined within the inorganic perovskite framework. Due to strong Coulombic interactions, these species retain their original excitonic character and form self-trapped polaron–excitons acting as radiative colour centres. These findings are expected to be relevant for a broad class of white-light emitting perovskites with large polaron relaxation energy. NRF (Natl Research Foundation, S’pore) MOE (Min. of Education, S’pore) Accepted version 2017-08-02T03:10:40Z 2019-12-06T14:52:34Z 2017-08-02T03:10:40Z 2019-12-06T14:52:34Z 2017 Journal Article Cortecchia, D., Yin, J., Bruno, A., Lo, S.-Z. A., Gurzadyan, G. G., Mhaisalkar, S., et al. (2017). Polaron self-localization in white-light emitting hybrid perovskites. Journal of Materials Chemistry C, 5(11), 2771-2780. 2050-7526 https://hdl.handle.net/10356/82288 http://hdl.handle.net/10220/43518 10.1039/C7TC00366H en Journal of Materials Chemistry C © 2017 The Royal Society of Chemistry. This is the author created version of a work that has been peer reviewed and accepted for publication by Journal of Materials Chemistry C, The Royal Society of Chemistry. It incorporates referee’s comments but changes resulting from the publishing process, such as copyediting, structural formatting, may not be reflected in this document. The published version is available at: [http://dx.doi.org/10.1039/C7TC00366H]. 34 p. application/pdf
spellingShingle Two-dimensional perovskites
White-light emitting perovskites
Cortecchia, Daniele
Yin, Jun
Bruno, Annalisa
Lo, Shu-Zee Alencious
Gurzadyan, Gagik G.
Mhaisalkar, Subodh
Brédas, Jean-Luc
Soci, Cesare
Polaron self-localization in white-light emitting hybrid perovskites
title Polaron self-localization in white-light emitting hybrid perovskites
title_full Polaron self-localization in white-light emitting hybrid perovskites
title_fullStr Polaron self-localization in white-light emitting hybrid perovskites
title_full_unstemmed Polaron self-localization in white-light emitting hybrid perovskites
title_short Polaron self-localization in white-light emitting hybrid perovskites
title_sort polaron self localization in white light emitting hybrid perovskites
topic Two-dimensional perovskites
White-light emitting perovskites
url https://hdl.handle.net/10356/82288
http://hdl.handle.net/10220/43518
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