Transient absorption (TA) spectroscopy is one of the most popular experimental methods to measure the excited state lifetimes and charge carrier recombination mechanisms in two dimensional (2D) semiconductors. This fundamental information is essential for designing and optimizing the next generation of ultrathin and lightweight 2D semiconductor-based optoelectronic devices. However, the interpretation of TA spectroscopy data varies across the community. The community lacks a unifying physical explanation for how and why experimental variables such as incident light intensity, sample-substrate interactions, and/or applied bias affect TA spectral data. This Perspective (1) compares the physical chemistry TA literature to nanomaterial physics literature from a historical perspective, (2) reviews multiple physical explanations that the TA community developed to explain spectral features and experimental trends, (3) provides a unifying explanation for how and why trions—and, more generally, Fermi polarons—contribute to TA spectra, and (4) quantifies the extent to which various physical interpretations and data analysis procedures yield different timescales and mechanisms for the same set of experimental results. We highlight the importance of considering trions/Fermi polarons in TA measurements and their implications for advancing our understanding of 2D material properties.
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21 November 2024
Perspective|
November 15 2024
Hiding in plain sight: The prevalence and impact of trions and Fermi polarons in transient absorption spectroscopy experiments of 2D semiconductors
Rachelle Austin
;
Rachelle Austin
(Conceptualization, Formal analysis, Writing – original draft, Writing – review & editing)
1
Department of Chemistry, Colorado State University
, Fort Collins, Colorado 80523, USA
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Tom Sayer
;
Tom Sayer
(Writing – review & editing)
2
Department of Chemistry, University of Colorado Boulder
, Boulder, Colorado 80302, USA
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Yusef Farah;
Yusef Farah
(Writing – review & editing)
1
Department of Chemistry, Colorado State University
, Fort Collins, Colorado 80523, USA
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Andrés Montoya-Castillo
;
Andrés Montoya-Castillo
(Conceptualization, Writing – original draft, Writing – review & editing)
2
Department of Chemistry, University of Colorado Boulder
, Boulder, Colorado 80302, USA
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Amber T. Krummel
;
Amber T. Krummel
(Conceptualization, Writing – original draft, Writing – review & editing)
1
Department of Chemistry, Colorado State University
, Fort Collins, Colorado 80523, USA
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Justin B. Sambur
Justin B. Sambur
a)
(Conceptualization, Writing – original draft, Writing – review & editing)
1
Department of Chemistry, Colorado State University
, Fort Collins, Colorado 80523, USA
3
School of Advanced Materials Discovery, Colorado State University
, Fort Collins, Colorado 80523, USA
a)Author to whom correspondence should be addressed: Justin.Sambur@colostate.edu
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a)Author to whom correspondence should be addressed: Justin.Sambur@colostate.edu
J. Chem. Phys. 161, 190901 (2024)
Article history
Received:
June 04 2024
Accepted:
September 23 2024
Citation
Rachelle Austin, Tom Sayer, Yusef Farah, Andrés Montoya-Castillo, Amber T. Krummel, Justin B. Sambur; Hiding in plain sight: The prevalence and impact of trions and Fermi polarons in transient absorption spectroscopy experiments of 2D semiconductors. J. Chem. Phys. 21 November 2024; 161 (19): 190901. https://doi.org/10.1063/5.0221956
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