Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy

Carrier diffusion and surface recombination are key processes influencing the performance of conventional semiconductor devices. However, the interplay of photon recycling together with these processes in halide perovskites obfuscates our understanding. Herein, we discern these inherent processes in...

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Main Authors: Feng, Minjun, Ye, Senyun, Guo, Yuanyuan, Sum, Tze Chien
Other Authors: School of Physical and Mathematical Sciences
Format: Journal Article
Language:English
Published: 2022
Subjects:
Online Access:https://hdl.handle.net/10356/161861
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author Feng, Minjun
Ye, Senyun
Guo, Yuanyuan
Sum, Tze Chien
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Feng, Minjun
Ye, Senyun
Guo, Yuanyuan
Sum, Tze Chien
author_sort Feng, Minjun
collection NTU
description Carrier diffusion and surface recombination are key processes influencing the performance of conventional semiconductor devices. However, the interplay of photon recycling together with these processes in halide perovskites obfuscates our understanding. Herein, we discern these inherent processes in a thin FAPbBr3 perovskite single crystal (PSC) utilizing a unique transient reflectance technique that allows accurate diffusion modeling with clear boundary conditions. Temperature-dependent measurements reveal the coexistence of shallow and deep traps at the surface. The inverse quadratic dependence of temperature on carrier mobility μ suggests an underlying scattering mechanism arising from the anharmonic deformation of the PbBr6 cage. Our findings ascertain the fundamental limits of the intrinsic surface recombination velocity (S) and carrier diffusion coefficient (D) in PSC samples. Importantly, these insights will help resolve the ongoing debate and clarify the ambiguity surrounding the contributions of photon recycling and carrier diffusion in perovskite optoelectronics.
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spelling ntu-10356/1618612023-02-28T20:01:38Z Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy Feng, Minjun Ye, Senyun Guo, Yuanyuan Sum, Tze Chien School of Physical and Mathematical Sciences Science::Physics::Optics and light Transient Reflectance Carrier Diffusion Surface Recombination Photon Recycling Perovskite Single Crystals Carrier diffusion and surface recombination are key processes influencing the performance of conventional semiconductor devices. However, the interplay of photon recycling together with these processes in halide perovskites obfuscates our understanding. Herein, we discern these inherent processes in a thin FAPbBr3 perovskite single crystal (PSC) utilizing a unique transient reflectance technique that allows accurate diffusion modeling with clear boundary conditions. Temperature-dependent measurements reveal the coexistence of shallow and deep traps at the surface. The inverse quadratic dependence of temperature on carrier mobility μ suggests an underlying scattering mechanism arising from the anharmonic deformation of the PbBr6 cage. Our findings ascertain the fundamental limits of the intrinsic surface recombination velocity (S) and carrier diffusion coefficient (D) in PSC samples. Importantly, these insights will help resolve the ongoing debate and clarify the ambiguity surrounding the contributions of photon recycling and carrier diffusion in perovskite optoelectronics. Ministry of Education (MOE) National Research Foundation (NRF) Submitted/Accepted version This research/project is supported by the Ministry of Education under its AcRF Tier 2 grants (MOE2019-T2-1-006, MOE2019-T2-1-097 and MOE-T2EP50120-0004); and the National Research Foundation (NRF) Singapore under its NRF Investigatorship (NRF-NRFI-2018-04). 2022-09-22T04:53:14Z 2022-09-22T04:53:14Z 2022 Journal Article Feng, M., Ye, S., Guo, Y. & Sum, T. C. (2022). Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy. Nano Letters, 22(17), 7195-7202. https://dx.doi.org/10.1021/acs.nanolett.2c02511 1530-6984 https://hdl.handle.net/10356/161861 10.1021/acs.nanolett.2c02511 35976688 2-s2.0-85136629584 17 22 7195 7202 en MOE2019-T2-1-006 MOE2019-T2-1-097 MOE-T2EP50120-0004 NRF-NRFI-2018-04 Nano Letters 10.21979/N9/8JDYHO This document is the Accepted Manuscript version of a Published Work that appeared in final form in Nano Letters, copyright © 2022 American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.nanolett.2c02511. application/pdf application/pdf
spellingShingle Science::Physics::Optics and light
Transient Reflectance
Carrier Diffusion
Surface Recombination
Photon Recycling
Perovskite Single Crystals
Feng, Minjun
Ye, Senyun
Guo, Yuanyuan
Sum, Tze Chien
Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy
title Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy
title_full Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy
title_fullStr Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy
title_full_unstemmed Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy
title_short Intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy
title_sort intrinsic carrier diffusion in perovskite thin films uncovered by transient reflectance spectroscopy
topic Science::Physics::Optics and light
Transient Reflectance
Carrier Diffusion
Surface Recombination
Photon Recycling
Perovskite Single Crystals
url https://hdl.handle.net/10356/161861
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AT guoyuanyuan intrinsiccarrierdiffusioninperovskitethinfilmsuncoveredbytransientreflectancespectroscopy
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