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Ultrafast Carrier Dynamics in Methylammonium Lead Iodide (MAPbI3) Perovskite Thin Films With Coexisting Orthorhombic and Tetragonal Phases

Li, Yong LU ; Yao, Zehan LU ; Jiao, Chenxu ; Wang, Zhengjun LU ; Schlawin, Frank and Baranov, Dmitry LU orcid (2026) In Small Structures 7(6).
Abstract

Methylammonium lead iodide (MAPbI3) is a prototypical soft-lattice semiconductor whose orthorhombic and tetragonal polymorphs can coexist and interconvert under optical excitation or changes in temperature. The mixed-phase regime attracts attention because of the carrier transfer between phases, which enables optoelectronic functionalities such as optical gain. Here, we investigate carrier dynamics in mixed-phase MAPbI3 thin films by comparing laser-induced phase coexistence at 77 K using time-resolved photoluminescence with thermally-induced phase coexistence at 148 K using transient absorption (TA) spectroscopy. By using low-repetition-rate TA to mitigate cumulative heating and avoid thermally induced phase... (More)

Methylammonium lead iodide (MAPbI3) is a prototypical soft-lattice semiconductor whose orthorhombic and tetragonal polymorphs can coexist and interconvert under optical excitation or changes in temperature. The mixed-phase regime attracts attention because of the carrier transfer between phases, which enables optoelectronic functionalities such as optical gain. Here, we investigate carrier dynamics in mixed-phase MAPbI3 thin films by comparing laser-induced phase coexistence at 77 K using time-resolved photoluminescence with thermally-induced phase coexistence at 148 K using transient absorption (TA) spectroscopy. By using low-repetition-rate TA to mitigate cumulative heating and avoid thermally induced phase conversion, we resolve the distinct spectral fingerprints of the orthorhombic and tetragonal phases and identify two carrier-transfer timescales of 36 and 539 ps, attributed to interfacial and bulk-mediated transfer, respectively. Despite carrier funneling in the mixed phase and high carrier densities, these conditions do not inherently lead to observable optical gain in the studied films.

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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
carrier transfer, halide perovskites, low-temperature photophysics, methylammonium lead iodide (MAPbI), orthorhombic-tetragonal transition, phase coexistence, time-resolved photoluminescence, transient absorption spectroscopy
in
Small Structures
volume
7
issue
6
article number
e70515
publisher
Wiley
external identifiers
  • scopus:105042225417
ISSN
2688-4062
DOI
10.1002/sstr.70515
project
Nanocrystal Solids for Quantum Technology
Tennbaserade nanostrukturer för optisk kvantteknologi
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2026 The Author(s). Small Structures published by Wiley-VCH GmbH.
id
494342d0-472d-41c2-a12f-791ab9a3a284
date added to LUP
2026-06-26 17:12:52
date last changed
2026-06-29 08:25:48
@article{494342d0-472d-41c2-a12f-791ab9a3a284,
  abstract     = {{<p>Methylammonium lead iodide (MAPbI<sub>3</sub>) is a prototypical soft-lattice semiconductor whose orthorhombic and tetragonal polymorphs can coexist and interconvert under optical excitation or changes in temperature. The mixed-phase regime attracts attention because of the carrier transfer between phases, which enables optoelectronic functionalities such as optical gain. Here, we investigate carrier dynamics in mixed-phase MAPbI<sub>3</sub> thin films by comparing laser-induced phase coexistence at 77 K using time-resolved photoluminescence with thermally-induced phase coexistence at 148 K using transient absorption (TA) spectroscopy. By using low-repetition-rate TA to mitigate cumulative heating and avoid thermally induced phase conversion, we resolve the distinct spectral fingerprints of the orthorhombic and tetragonal phases and identify two carrier-transfer timescales of 36 and 539 ps, attributed to interfacial and bulk-mediated transfer, respectively. Despite carrier funneling in the mixed phase and high carrier densities, these conditions do not inherently lead to observable optical gain in the studied films.</p>}},
  author       = {{Li, Yong and Yao, Zehan and Jiao, Chenxu and Wang, Zhengjun and Schlawin, Frank and Baranov, Dmitry}},
  issn         = {{2688-4062}},
  keywords     = {{carrier transfer; halide perovskites; low-temperature photophysics; methylammonium lead iodide (MAPbI); orthorhombic-tetragonal transition; phase coexistence; time-resolved photoluminescence; transient absorption spectroscopy}},
  language     = {{eng}},
  number       = {{6}},
  publisher    = {{Wiley}},
  series       = {{Small Structures}},
  title        = {{Ultrafast Carrier Dynamics in Methylammonium Lead Iodide (MAPbI<sub>3</sub>) Perovskite Thin Films With Coexisting Orthorhombic and Tetragonal Phases}},
  url          = {{http://dx.doi.org/10.1002/sstr.70515}},
  doi          = {{10.1002/sstr.70515}},
  volume       = {{7}},
  year         = {{2026}},
}