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Physics > Chemical Physics
Title: Determining Quasi-Equilibrium Electron and Hole Distributions of Plasmonic Photocatalysts using Photomodulated X-ray Absorption Spectroscopy
(Submitted on 30 Aug 2023 (v1), last revised 24 Jan 2024 (this version, v2))
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.
Submission history
From: Levi Palmer [view email][v1] Wed, 30 Aug 2023 05:33:21 GMT (1809kb)
[v2] Wed, 24 Jan 2024 20:15:21 GMT (4469kb)
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