Layered multiple scattering approach to Hard X-ray photoelectron diffraction: theory and application

Abstract Photoelectron diffraction (PED) is a powerful technique for resolving surface structures with sub-angstrom precision. At high photon energies, angle-resolved photoemission spectroscopy (ARPES) reveals PED effects, often challenged by small cross-sections, momentum transfer, and phonon scatt...

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Main Authors: Trung-Phuc Vo, Olena Tkach, Sylvain Tricot, Didier Sébilleau, Jürgen Braun, Aki Pulkkinen, Aimo Winkelmann, Olena Fedchenko, Yaryna Lytvynenko, Dmitry Vasilyev, Hans-Joachim Elmers, Gerd Schönhense, Ján Minár
Format: Article
Language:English
Published: Nature Portfolio 2025-05-01
Series:npj Computational Materials
Online Access:https://doi.org/10.1038/s41524-025-01653-y
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Summary:Abstract Photoelectron diffraction (PED) is a powerful technique for resolving surface structures with sub-angstrom precision. At high photon energies, angle-resolved photoemission spectroscopy (ARPES) reveals PED effects, often challenged by small cross-sections, momentum transfer, and phonon scattering. X-ray PED (XPD) is not only an advantageous approach but also exhibits unexpected effects. We present a PED implementation for the spin-polarized relativistic Korringa-Kohn-Rostoker (SPRKKR) package to disentangle them, employing multiple scattering theory and a one-step photoemission model. Unlike conventional real-space approaches, our method uses a k-space formulation via the layer-KKR method, offering efficient and accurate calculations across a wide energy range (20-8000 eV) without angular momentum or cluster size convergence issues. Additionally, the alloy analogy model enables simulations of finite-temperature XPD and effects in soft/hard X-ray ARPES. Applications include modeling circular dichroism in angular distributions (CDAD) in core-level photoemission of Si(100) 2p and Ge(100) 3p, excited by 6000 eV photons with circular polarization.
ISSN:2057-3960