1. Determining Quasi-Equilibrium Electron and Hole Distributions of Plasmonic Photocatalysts using Photomodulated X-ray Absorption Spectroscopy
- Author
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Palmer, Levi D., Lee, Wonseok, Dong, Chung Li, Liu, Ru-Shi, Wu, Nianqiang, and Cushing, Scott K.
- Subjects
Physics - Chemical Physics ,Condensed Matter - Materials Science ,Physics - Optics - Abstract
Most photocatalytic and photovoltaic devices operate under broadband, constant illumination. Electron and hole dynamics in these devices, however, are usually measured using ultrafast pulsed lasers in a narrow wavelength range. In this work, we prove that steady-state, photomodulated X-ray spectra from a non-time-resolved synchrotron beamline can be used to estimate electron and hole distributions. A set of plasmonic metal core-shell nanoparticles is designed to systematically isolate photothermal, hot electron, and thermalized electron-hole pairs in a TiO2 shell. Steady-state changes in the Ti L2,3 edge are measured with and without continuous-wave illumination of the nanoparticle's localized surface plasmon resonance. Ab initio excited-state X-ray theory developed for transient X-ray measurements is then applied to model the experimental spectra in an attempt to extract the resultant steady-state carrier distributions. The results suggest that, within error, the quasi-equilibrium carrier distribution can be determined even from relatively noisy data with mixed excited-state phenomena., Comment: 41 pages, 18 figures
- Published
- 2023
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