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Optimizing the quasi-equilibrium state of hot carriers in all-inorganic lead halide perovskite nanocrystals through Mn doping : fundamental dynamics and device perspectives

Meng, Jie ; Lan, Zhenyun ; Lin, Weihua LU ; Liang, Mingli ; Zou, Xianshao LU ; Zhao, Qian ; Geng, Huifang LU ; Castelli, Ivano E. ; Canton, Sophie E. LU and Pullerits, Tönu LU , et al. (2022) In Chemical Science 13(6). p.1734-1745
Abstract

Hot carrier (HC) cooling accounts for the significant energy loss in lead halide perovskite (LHP) solar cells. Here, we study HC relaxation dynamics in Mn-doped LHP CsPbI3 nanocrystals (NCs), combining transient absorption spectroscopy and density functional theory (DFT) calculations. We demonstrate that Mn2+ doping (1) enlarges the longitudinal optical (LO)-acoustic phonon bandgap, (2) enhances the electron-LO phonon coupling strength, and (3) adds HC relaxation pathways via Mn orbitals within the bands. The spectroscopic study shows that the HC cooling process is decelerated after doping under band-edge excitation due to the dominant phonon bandgap enlargement. When the excitation photon energy is larger than the optical bandgap and... (More)

Hot carrier (HC) cooling accounts for the significant energy loss in lead halide perovskite (LHP) solar cells. Here, we study HC relaxation dynamics in Mn-doped LHP CsPbI3 nanocrystals (NCs), combining transient absorption spectroscopy and density functional theory (DFT) calculations. We demonstrate that Mn2+ doping (1) enlarges the longitudinal optical (LO)-acoustic phonon bandgap, (2) enhances the electron-LO phonon coupling strength, and (3) adds HC relaxation pathways via Mn orbitals within the bands. The spectroscopic study shows that the HC cooling process is decelerated after doping under band-edge excitation due to the dominant phonon bandgap enlargement. When the excitation photon energy is larger than the optical bandgap and the Mn2+ transition gap, the doping accelerates the cooling rate owing to the dominant effect of enhanced carrier-phonon coupling and relaxation pathways. We demonstrate that such a phenomenon is optimal for the application of hot carrier solar cells. The enhanced electron-LO phonon coupling and accelerated cooling of high-temperature hot carriers efficiently establish a high-temperature thermal quasi-equilibrium where the excessive energy of the hot carriers is transferred to heat the cold carriers. On the other hand, the enlarged phononic band-gap prevents further cooling of such a quasi-equilibrium, which facilitates the energy conversion process. Our results manifest a straightforward methodology to optimize the HC dynamics for hot carrier solar cells by element doping. This journal is

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Chemical Science
volume
13
issue
6
pages
12 pages
publisher
Royal Society of Chemistry
external identifiers
  • pmid:35282633
  • scopus:85124685628
ISSN
2041-6520
DOI
10.1039/d1sc05799e
language
English
LU publication?
yes
id
3d4bab90-27a2-433f-ac02-512cac0aec9e
date added to LUP
2022-05-18 15:36:29
date last changed
2025-03-21 16:49:11
@article{3d4bab90-27a2-433f-ac02-512cac0aec9e,
  abstract     = {{<p>Hot carrier (HC) cooling accounts for the significant energy loss in lead halide perovskite (LHP) solar cells. Here, we study HC relaxation dynamics in Mn-doped LHP CsPbI3 nanocrystals (NCs), combining transient absorption spectroscopy and density functional theory (DFT) calculations. We demonstrate that Mn2+ doping (1) enlarges the longitudinal optical (LO)-acoustic phonon bandgap, (2) enhances the electron-LO phonon coupling strength, and (3) adds HC relaxation pathways via Mn orbitals within the bands. The spectroscopic study shows that the HC cooling process is decelerated after doping under band-edge excitation due to the dominant phonon bandgap enlargement. When the excitation photon energy is larger than the optical bandgap and the Mn2+ transition gap, the doping accelerates the cooling rate owing to the dominant effect of enhanced carrier-phonon coupling and relaxation pathways. We demonstrate that such a phenomenon is optimal for the application of hot carrier solar cells. The enhanced electron-LO phonon coupling and accelerated cooling of high-temperature hot carriers efficiently establish a high-temperature thermal quasi-equilibrium where the excessive energy of the hot carriers is transferred to heat the cold carriers. On the other hand, the enlarged phononic band-gap prevents further cooling of such a quasi-equilibrium, which facilitates the energy conversion process. Our results manifest a straightforward methodology to optimize the HC dynamics for hot carrier solar cells by element doping. This journal is </p>}},
  author       = {{Meng, Jie and Lan, Zhenyun and Lin, Weihua and Liang, Mingli and Zou, Xianshao and Zhao, Qian and Geng, Huifang and Castelli, Ivano E. and Canton, Sophie E. and Pullerits, Tönu and Zheng, Kaibo}},
  issn         = {{2041-6520}},
  language     = {{eng}},
  month        = {{02}},
  number       = {{6}},
  pages        = {{1734--1745}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Chemical Science}},
  title        = {{Optimizing the quasi-equilibrium state of hot carriers in all-inorganic lead halide perovskite nanocrystals through Mn doping : fundamental dynamics and device perspectives}},
  url          = {{http://dx.doi.org/10.1039/d1sc05799e}},
  doi          = {{10.1039/d1sc05799e}},
  volume       = {{13}},
  year         = {{2022}},
}