The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites

Two-dimensional (2D) lead halide Ruddlesden–Popper perovskites (RPP) have recently emerged as a prospective material system for optoelectronic applications. Their self-assembled multi quantum-well structure gives rise to the novel interwell energy funnelling phenomenon, which is of broad interests f...

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Main Authors: Giovanni, David, Ramesh, Sankaran, Righetto, Marcello, Lim, Melvin Jia Wei, Zhang, Qiannan, Wang, Yue, Ye, Senyun, Xu, Qiang, Mathews, Nripan, Sum, Tze Chien
Other Authors: School of Physical and Mathematical Sciences
Format: Journal Article
Language:English
Published: 2021
Subjects:
Online Access:https://hdl.handle.net/10356/147025
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author Giovanni, David
Ramesh, Sankaran
Righetto, Marcello
Lim, Melvin Jia Wei
Zhang, Qiannan
Wang, Yue
Ye, Senyun
Xu, Qiang
Mathews, Nripan
Sum, Tze Chien
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Giovanni, David
Ramesh, Sankaran
Righetto, Marcello
Lim, Melvin Jia Wei
Zhang, Qiannan
Wang, Yue
Ye, Senyun
Xu, Qiang
Mathews, Nripan
Sum, Tze Chien
author_sort Giovanni, David
collection NTU
description Two-dimensional (2D) lead halide Ruddlesden–Popper perovskites (RPP) have recently emerged as a prospective material system for optoelectronic applications. Their self-assembled multi quantum-well structure gives rise to the novel interwell energy funnelling phenomenon, which is of broad interests for photovoltaics, light-emission applications, and emerging technologies (e.g., spintronics). Herein, we develop a realistic finite quantum-well superlattice model that corroborates the hypothesis of exciton delocalization across different quantum-wells in RPP. Such delocalization leads to a sub-50 fs coherent energy transfer between adjacent wells, with the efficiency depending on the RPP phase matching and the organic large cation barrier lengths. Our approach provides a coherent and comprehensive account for both steady-state and transient dynamical experimental results in RPPs. Importantly, these findings pave the way for a deeper understanding of these systems, as a cornerstone crucial for establishing material design rules to realize efficient RPP-based devices.
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spelling ntu-10356/1470252023-02-28T19:50:26Z The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites Giovanni, David Ramesh, Sankaran Righetto, Marcello Lim, Melvin Jia Wei Zhang, Qiannan Wang, Yue Ye, Senyun Xu, Qiang Mathews, Nripan Sum, Tze Chien School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) SPMS, Department of Physics and Applied Physics (PAP) Energy Research Institute @ NTU (ERI@N) Science::Physics::Optics and light Engineering::Materials::Photonics and optoelectronics materials Excitons Binding Energy Two-dimensional (2D) lead halide Ruddlesden–Popper perovskites (RPP) have recently emerged as a prospective material system for optoelectronic applications. Their self-assembled multi quantum-well structure gives rise to the novel interwell energy funnelling phenomenon, which is of broad interests for photovoltaics, light-emission applications, and emerging technologies (e.g., spintronics). Herein, we develop a realistic finite quantum-well superlattice model that corroborates the hypothesis of exciton delocalization across different quantum-wells in RPP. Such delocalization leads to a sub-50 fs coherent energy transfer between adjacent wells, with the efficiency depending on the RPP phase matching and the organic large cation barrier lengths. Our approach provides a coherent and comprehensive account for both steady-state and transient dynamical experimental results in RPPs. Importantly, these findings pave the way for a deeper understanding of these systems, as a cornerstone crucial for establishing material design rules to realize efficient RPP-based devices. Ministry of Education (MOE) Nanyang Technological University National Research Foundation (NRF) Accepted version This research was supported by Nanyang Technological University under its start-up grant (M4080514); the Ministry of Education under its AcRF Tier 1 grant (RG91/19) and Tier 2 grants (MOE2016-T2-1-034, MOE2017-T2-1-001 and MOE2017-T2-2-002); and the National Research Foundation (NRF) Singapore under its Competitive Research Program (NRF-CRP14-2014-03) and its NRF Investigatorship (NRF-NRFI-2018-04). 2021-03-22T06:36:07Z 2021-03-22T06:36:07Z 2021 Journal Article Giovanni, D., Ramesh, S., Righetto, M., Lim, M. J. W., Zhang, Q., Wang, Y., Ye, S., Xu, Q., Mathews, N. & Sum, T. C. (2021). The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites. Nano Letters, 21(1), 405-413. https://dx.doi.org/10.1021/acs.nanolett.0c03800 1530-6992 https://hdl.handle.net/10356/147025 10.1021/acs.nanolett.0c03800 1 21 405 413 en NTU Start-up Grant M4080514 RG91/19 MOE2016-T2-1-034 MOE2017-T2-1-001 MOE2017-T2-2-002 NRF-CRP14-2014-03 NRF-NRFI-2018-04 Nano Letters https://doi.org/10.21979/N9/OIYOW1 This document is the Accepted Manuscript version of a Published Work that appeared in final form in Nano Letters, copyright © 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.0c03800 application/pdf application/pdf
spellingShingle Science::Physics::Optics and light
Engineering::Materials::Photonics and optoelectronics materials
Excitons
Binding Energy
Giovanni, David
Ramesh, Sankaran
Righetto, Marcello
Lim, Melvin Jia Wei
Zhang, Qiannan
Wang, Yue
Ye, Senyun
Xu, Qiang
Mathews, Nripan
Sum, Tze Chien
The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites
title The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites
title_full The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites
title_fullStr The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites
title_full_unstemmed The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites
title_short The physics of interlayer exciton delocalization in Ruddlesden–Popper lead halide perovskites
title_sort physics of interlayer exciton delocalization in ruddlesden popper lead halide perovskites
topic Science::Physics::Optics and light
Engineering::Materials::Photonics and optoelectronics materials
Excitons
Binding Energy
url https://hdl.handle.net/10356/147025
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