https://scholars.lib.ntu.edu.tw/handle/123456789/641876
標題: | Determining Quasi-Equilibrium Electron and Hole Distributions of Plasmonic Photocatalysts Using Photomodulated X-ray Absorption Spectroscopy | 作者: | Palmer, Levi Daniel Lee, Wonseok Dong, Chung-Li RU-SHI LIU Wu, Nianqiang Cushing, Scott Kevin |
關鍵字: | Bethe-Salpeter equation; X-ray absorption; X-ray spectroscopy; core−shell nanoparticles; hot carriers; photocatalysis; plasmonics | 公開日期: | 2-四月-2024 | 卷: | 18 | 期: | 13 | 起(迄)頁: | 9344 | 來源出版物: | ACS nano | 摘要: | Most photocatalytic and photovoltaic devices operate under broadband, constant illumination. Electron and hole dynamics in these devices, however, are usually measured by using ultrafast pulsed lasers in a narrow wavelength range. In this work, we use excited-state X-ray theory originally developed for transient X-ray experiments to study steady-state photomodulated X-ray spectra. We use this method to attempt to extract electron and hole distributions from spectra collected at a nontime-resolved synchrotron beamline. A set of plasmonic metal core-shell nanoparticles is designed as the control experiment because they can 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. The results suggest that within error the quasi-equilibrium carrier distribution can be determined even from relatively noisy data with mixed excited-state phenomena. Just as importantly, the theoretical analysis of noisy data is used to provide guidelines for the beamline development of photomodulated steady-state spectroscopy. |
URI: | https://scholars.lib.ntu.edu.tw/handle/123456789/641876 | ISSN: | 19360851 | DOI: | 10.1021/acsnano.3c08181 |
顯示於: | 化學系 |
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