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Unveiling Mechanism of Temperature-Dependent Self-Trapped Exciton Emission in 1D Hybrid Organic–Inorganic Tin Halide for Advanced Thermography

He, Yanmei LU ; Cai, Xinyi ; Wang, Xiaochen ; Liisberg, Mikkel Baldtzer ; Dostál, Jakub LU ; Zhang, Muyi ; Kloz, Miroslav ; Gao, Feng ; Pullerits, Tönu LU and Chen, Junsheng LU (2025) In Advanced Optical Materials 13(2).
Abstract

Lead-free hybrid metal halide phosphors/crystals showing self-trapped exciton (STE) emission have been recently explored for thermography due to the strong temperature dependence of their photoluminescence (PL) lifetime (τ). However, realizing high-spatial-resolution thermography using polycrystalline powders or crystals presents a challenge. Moreover, the underlying mechanism of temperature-dependent STE remains elusive. Herein, a homogeneous 1D ODASn2I6 (ODA, 1,8-octanediamine) nm-scale thin film exhibiting efficient STE emission is investigated. The PL decay shows a strong temperature dependence from 275 K (τ ≈ 1.31 µs) to 350 K (τ ≈ 0.65 µs) yielding a thermal sensitivity of 0.014 K−1. By employing... (More)

Lead-free hybrid metal halide phosphors/crystals showing self-trapped exciton (STE) emission have been recently explored for thermography due to the strong temperature dependence of their photoluminescence (PL) lifetime (τ). However, realizing high-spatial-resolution thermography using polycrystalline powders or crystals presents a challenge. Moreover, the underlying mechanism of temperature-dependent STE remains elusive. Herein, a homogeneous 1D ODASn2I6 (ODA, 1,8-octanediamine) nm-scale thin film exhibiting efficient STE emission is investigated. The PL decay shows a strong temperature dependence from 275 K (τ ≈ 1.31 µs) to 350 K (τ ≈ 0.65 µs) yielding a thermal sensitivity of 0.014 K−1. By employing temperature-dependent transient absorption spectroscopy, detailed information is obtained about the relaxation processes prior to the STE formation. Simultaneous analyses of steady-state and time-resolved spectroscopies lead to a self-consistent model where the thermally activated phonon-assisted nonradiative pathway explains the temperature dependence of the PL lifetime via a conical intersection between the ground state and STE potential energy surfaces. Finally, a discernible 50 ns variation in PL lifetimes across different heated regimes over a distance of 1.15 mm is successfully demonstrated with fluorescence lifetime imaging microscopy, underscoring the substantial potential of ODASn2I6 thin film for high-spatial-resolution thermography.

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author
; ; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
exciton dynamics, hybrid organic–inorganic tin halide, self-trapped exciton, thermography, ultrafast spectroscopy
in
Advanced Optical Materials
volume
13
issue
2
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:85206929562
ISSN
2195-1071
DOI
10.1002/adom.202402061
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2024 The Author(s). Advanced Optical Materials published by Wiley-VCH GmbH.
id
4b911f12-a5b3-4a03-97ff-20b5429b4824
date added to LUP
2024-11-01 10:52:38
date last changed
2025-04-04 14:30:46
@article{4b911f12-a5b3-4a03-97ff-20b5429b4824,
  abstract     = {{<p>Lead-free hybrid metal halide phosphors/crystals showing self-trapped exciton (STE) emission have been recently explored for thermography due to the strong temperature dependence of their photoluminescence (PL) lifetime (τ). However, realizing high-spatial-resolution thermography using polycrystalline powders or crystals presents a challenge. Moreover, the underlying mechanism of temperature-dependent STE remains elusive. Herein, a homogeneous 1D ODASn<sub>2</sub>I<sub>6</sub> (ODA, 1,8-octanediamine) nm-scale thin film exhibiting efficient STE emission is investigated. The PL decay shows a strong temperature dependence from 275 K (τ ≈ 1.31 µs) to 350 K (τ ≈ 0.65 µs) yielding a thermal sensitivity of 0.014 K<sup>−1</sup>. By employing temperature-dependent transient absorption spectroscopy, detailed information is obtained about the relaxation processes prior to the STE formation. Simultaneous analyses of steady-state and time-resolved spectroscopies lead to a self-consistent model where the thermally activated phonon-assisted nonradiative pathway explains the temperature dependence of the PL lifetime via a conical intersection between the ground state and STE potential energy surfaces. Finally, a discernible 50 ns variation in PL lifetimes across different heated regimes over a distance of 1.15 mm is successfully demonstrated with fluorescence lifetime imaging microscopy, underscoring the substantial potential of ODASn<sub>2</sub>I<sub>6</sub> thin film for high-spatial-resolution thermography.</p>}},
  author       = {{He, Yanmei and Cai, Xinyi and Wang, Xiaochen and Liisberg, Mikkel Baldtzer and Dostál, Jakub and Zhang, Muyi and Kloz, Miroslav and Gao, Feng and Pullerits, Tönu and Chen, Junsheng}},
  issn         = {{2195-1071}},
  keywords     = {{exciton dynamics; hybrid organic–inorganic tin halide; self-trapped exciton; thermography; ultrafast spectroscopy}},
  language     = {{eng}},
  number       = {{2}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Advanced Optical Materials}},
  title        = {{Unveiling Mechanism of Temperature-Dependent Self-Trapped Exciton Emission in 1D Hybrid Organic–Inorganic Tin Halide for Advanced Thermography}},
  url          = {{http://dx.doi.org/10.1002/adom.202402061}},
  doi          = {{10.1002/adom.202402061}},
  volume       = {{13}},
  year         = {{2025}},
}