Kavli Affiliate: Scott K. Cushing
| First 5 Authors: Hanzhe Liu, Jonathan M. Michelsen, Isabel M. Klein, Scott K. Cushing,
| Summary:
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 $pm$ 40 fs. Holes are excited with an average
excess energy of ~1 eV and thermalize in 1130 $pm$ 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.
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