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5 October 2015 Exploring the time-scale of photo-initiated interfacial electron transfer through first-principles interpretation of ultrafast X-ray spectroscopy (Presentation Recording)
David Prendergast, Sri Chaitanya Das Pemmaraju
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Proceedings Volume 9560, Solar Hydrogen and Nanotechnology X; 95600P (2015) https://doi.org/10.1117/12.2190444
Event: SPIE Optics + Photonics for Sustainable Energy, 2015, San Diego, California, United States
Abstract
With the advent of X-ray free electron lasers and table-top high-harmonic-generation X-ray sources, we can now explore changes in electronic structure on ultrafast time scales -- at or less than 1ps. Transient X-ray spectroscopy of this kind provides a direct probe of relevant electronic levels related to photoinitiated processes and associated interfacial electron transfer as the initial step in solar energy conversion. However, the interpretation of such spectra is typically fraught with difficulty, especially since we rarely have access to spectral standards for nonequilibrium states. To this end, direct first-principles simulations of X-ray absorption spectra can provide the necessary connection between measurements and reliable models of the atomic and electronic structure. We present examples of modeling excited states of materials interfaces relevant to solar harvesting and their corresponding X-ray spectra in either photoemission or absorption modalities. In this way, we can establish particular electron transfer mechanisms to reveal detailed working principles of materials systems in solar applications and provide insight for improved efficiency.
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David Prendergast and Sri Chaitanya Das Pemmaraju "Exploring the time-scale of photo-initiated interfacial electron transfer through first-principles interpretation of ultrafast X-ray spectroscopy (Presentation Recording)", Proc. SPIE 9560, Solar Hydrogen and Nanotechnology X, 95600P (5 October 2015); https://doi.org/10.1117/12.2190444
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KEYWORDS
X-rays
Spectroscopy
Ultrafast laser spectroscopy
Absorption
Systems modeling
Free electron lasers
Solar energy
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