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AbstractAbstract
[en] Highlights: • Ultrafast interfacial charge transfer is probed with atomic site specificity. • Femtosecond X-ray photoelectron spectroscopy using a free electron laser. • Efficient and flexible picosecond X-ray photoelectron pump–probe scheme using synchrotron radiation. - Abstract: X-ray photoelectron spectroscopy (XPS) is one of the most powerful techniques to quantitatively analyze the chemical composition and electronic structure of surfaces and interfaces in a non-destructive fashion. Extending this technique into the time domain has the exciting potential to shed new light on electronic and chemical dynamics at surfaces by revealing transient charge configurations with element- and site-specificity. Here, we describe prospects and challenges that are associated with the implementation of picosecond and femtosecond time-resolved X-ray photoelectron spectroscopy at third-generation synchrotrons and X-ray free-electron lasers, respectively. In particular, we discuss a series of laser-pump/X-ray-probe photoemission experiments performed on semiconductor surfaces, molecule-semiconductor interfaces, and films of semiconductor nanoparticles that demonstrate the high sensitivity of time-resolved XPS to light-induced charge carrier generation, diffusion and recombination within the space charge layers of these materials. Employing the showcase example of photo-induced electronic dynamics in a dye-sensitized semiconductor system, we highlight the unique possibility to probe heterogeneous charge transfer dynamics from both sides of an interface, i.e., from the perspective of the molecular electron donor and the semiconductor acceptor, simultaneously. Such capabilities will be crucial to improve our microscopic understanding of interfacial charge redistribution and associated chemical dynamics, which are at the heart of emerging energy conversion, solar fuel generation, and energy storage technologies.
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Source
S0368-2048(15)00059-6; Available from http://dx.doi.org/10.1016/j.elspec.2015.03.002; Copyright (c) 2015 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Record Type
Journal Article
Journal
Journal of Electron Spectroscopy and Related Phenomena; ISSN 0368-2048;
; CODEN JESRAW; v. 200; p. 64-77

Country of publication
BINDING ENERGY, CHARGE CARRIERS, CHEMICAL COMPOSITION, DEPLETION LAYER, ELECTRIC POTENTIAL, ELECTRONIC STRUCTURE, FREE ELECTRON LASERS, INTERFACES, NANOPARTICLES, OPTICAL PUMPING, PHOTOEMISSION, SEMICONDUCTOR MATERIALS, SPACE CHARGE, SURFACES, SYNCHROTRON RADIATION, SYNCHROTRONS, TIME RESOLUTION, X RADIATION, X-RAY PHOTOELECTRON SPECTROSCOPY
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