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Measuring photoexcited electron and hole dynamics in ZnTe and modeling excited state core-valence effects in transient XUV reflection spectroscopy

Liu, Hanzhe and Michelsen, Jonathan M. and Klein, Isabel M. and Cushing, Scott K. (2021) Measuring photoexcited electron and hole dynamics in ZnTe and modeling excited state core-valence effects in transient XUV reflection spectroscopy. . (Unpublished) https://resolver.caltech.edu/CaltechAUTHORS:20210831-203959863

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Abstract

Transient XUV spectroscopy is growing in popularity for the measurement of solar fuel and photovoltaic materials as it can separately measure electron and hole energies for multiple elements at once. However, interpretation of transient XUV measurements is complicated by changes in core-valence exciton and angular momentum effects after photoexcitation. Here, we report the photoexcited electron and hole dynamics for ZnTe, a promising material for CO₂ reduction, following 400 nm excitation. We apply a newly developed, ab-initio theoretical approach based on density functional theory and the Bethe-Salpeter equation to accurately predict the excited state change in the measured transient XUV spectra. Electrons excited to the conduction band are measured with a thermalization rate of 70 ± 40 fs. Holes are excited with an average excess energy of ~1 eV and thermalize in 1130 ± 150 fs. The theoretical approach also allows an estimated assignment of inter- and intra-valley relaxation pathways in k-space using the relative amplitudes of the core-valence excitons.


Item Type:Report or Paper (Discussion Paper)
Related URLs:
URLURL TypeDescription
http://arxiv.org/abs/2108.02262arXivDiscussion Paper
ORCID:
AuthorORCID
Liu, Hanzhe0000-0001-9001-725X
Cushing, Scott K.0000-0003-3538-2259
Additional Information:Attribution 4.0 International (CC BY 4.0)
Record Number:CaltechAUTHORS:20210831-203959863
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210831-203959863
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:110663
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:01 Sep 2021 14:30
Last Modified:01 Sep 2021 14:30

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