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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 wavelengthrange. In this work, we prove that steady-state, photomodulated X-ray spectrafrom a non-time-resolved synchrotron beamline can be used to estimate electronand hole distributions. A set of plasmonic metal core-shell nanoparticles isdesigned to systematically isolate photothermal, hot electron, and thermalizedelectron-hole pairs in a TiO2 shell. Steady-state changes in the Ti L2,3 edgeare measured with and without continuous-wave illumination of thenanoparticle's localized surface plasmon resonance. Ab initio excited-stateX-ray theory developed for transient X-ray measurements is then applied tomodel the experimental spectra in an attempt to extract the resultantsteady-state carrier distributions. The results suggest that, within error, thequasi-equilibrium carrier distribution can be determined even from relativelynoisy data with mixed excited-state phenomena.

Determining Quasi-Equilibrium Electron and Hole Distributions of Plasmonic Photocatalysts using Photomodulated X-ray Absorption Spectroscopy