Hiding in plain sight: The prevalence and impact of trions and Fermi polarons in transient absorption spectroscopy experiments of 2D semiconductors

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...

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Bibliographic Details
Published in:The Journal of chemical physics 2024-11, Vol.161 (19)
Main Authors: Austin, Rachelle, Sayer, Tom, Farah, Yusef, Montoya-Castillo, Andrés, Krummel, Amber T., Sambur, Justin B.
Format: Article
Language:English
Subjects:
Absorption spectroscopy
Carrier recombination
Current carriers
Data analysis
Excitation spectra
Incident light
Luminous intensity
Material properties
Nanomaterials
Optoelectronic devices
Physical chemistry
Polarons
Semiconductors
Trions
Two dimensional analysis
Two dimensional materials
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Summary: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.
ISSN:0021-9606
1089-7690
1089-7690
DOI:10.1063/5.0221956