All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites

We discuss a variety of many-body approaches, within effective-mass and k . p envelope-function formalisms, for calculating correlated single excitons in semiconductor nanocrystals (NCs) to all orders in the electron-hole Coulomb interaction. These approaches are applied to NCs of the lead-halid...

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Main Authors: Blundell, S. A., Guet, Claude
Other Authors: School of Physical and Mathematical Sciences
Format: Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/170803
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Institution: Nanyang Technological University
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spelling sg-ntu-dr.10356-1708032023-10-16T15:35:56Z All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites Blundell, S. A. Guet, Claude School of Physical and Mathematical Sciences Science::Physics Approximation Algorithms Halide Perovskites We discuss a variety of many-body approaches, within effective-mass and k . p envelope-function formalisms, for calculating correlated single excitons in semiconductor nanocrystals (NCs) to all orders in the electron-hole Coulomb interaction. These approaches are applied to NCs of the lead-halide perovskite CsPbBr3, which typically present excitons in intermediate confinement with physical observables often strongly renormalized by correlation (e.g., radiative decay rate enhanced by a factor of about 7 relative to a mean-field approach, for a NC of edge length 11 nm). The many-body methods considered include the particle-hole Bethe-Salpeter equation, configuration interaction with single excitations, and the random-phase approximation with exchange (RPAE), which are shown to be closely related to each other but to treat k . p corrections differently, with RPAE being the most complete method. The methods are applied to calculate the correlation energy, the radiative lifetime, and the long-range Coulomb contribution to the fine structure of the ground-state exciton. In the limit of large NC sizes, the numerical results are shown to agree well with analytical results for this limit, where these are known. Correlated excited states of the single exciton are used to calculate the one-photon absorption cross section; the shape of the resulting cross-section curve (versus laser wavelength) at threshold and up to an excitation energy of about 1 eV is in good agreement with experimental cross sections. The equations for the methods are explicitly adapted to spherical symmetry (involving radial integrals and angular factors) and in this form permit a rapid computation for systems in intermediate confinement. Published version 2023-10-10T08:23:28Z 2023-10-10T08:23:28Z 2022 Journal Article Blundell, S. A. & Guet, C. (2022). All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites. Physical Review B, 105(15), 155420-. https://dx.doi.org/10.1103/PhysRevB.105.155420 1098-0121 https://hdl.handle.net/10356/170803 10.1103/PhysRevB.105.155420 2-s2.0-85129428514 15 105 155420 en Physical Review B © 2022 American Physical Society. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1103/PhysRevB.105.155420 application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Physics
Approximation Algorithms
Halide Perovskites
spellingShingle Science::Physics
Approximation Algorithms
Halide Perovskites
Blundell, S. A.
Guet, Claude
All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites
description We discuss a variety of many-body approaches, within effective-mass and k . p envelope-function formalisms, for calculating correlated single excitons in semiconductor nanocrystals (NCs) to all orders in the electron-hole Coulomb interaction. These approaches are applied to NCs of the lead-halide perovskite CsPbBr3, which typically present excitons in intermediate confinement with physical observables often strongly renormalized by correlation (e.g., radiative decay rate enhanced by a factor of about 7 relative to a mean-field approach, for a NC of edge length 11 nm). The many-body methods considered include the particle-hole Bethe-Salpeter equation, configuration interaction with single excitations, and the random-phase approximation with exchange (RPAE), which are shown to be closely related to each other but to treat k . p corrections differently, with RPAE being the most complete method. The methods are applied to calculate the correlation energy, the radiative lifetime, and the long-range Coulomb contribution to the fine structure of the ground-state exciton. In the limit of large NC sizes, the numerical results are shown to agree well with analytical results for this limit, where these are known. Correlated excited states of the single exciton are used to calculate the one-photon absorption cross section; the shape of the resulting cross-section curve (versus laser wavelength) at threshold and up to an excitation energy of about 1 eV is in good agreement with experimental cross sections. The equations for the methods are explicitly adapted to spherical symmetry (involving radial integrals and angular factors) and in this form permit a rapid computation for systems in intermediate confinement.
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Blundell, S. A.
Guet, Claude
format Article
author Blundell, S. A.
Guet, Claude
author_sort Blundell, S. A.
title All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites
title_short All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites
title_full All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites
title_fullStr All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites
title_full_unstemmed All-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites
title_sort all-order correlation of single excitons in nanocrystals using a k . p envelope-function approach: application to lead-halide perovskites
publishDate 2023
url https://hdl.handle.net/10356/170803
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