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Main Title: Probing electron and hole colocalization by resonant four-wave mixing spectroscopy in the extreme ultraviolet
Author(s): Rottke, Horst
Engel, Robin Y.
Schick, Daniel
Schunck, Jan O.
Miedema, Piter S.
Borchert, Martin C.
Kuhlmann, Marion
Ekanayake, Nagitha
Dziarzhytski, Siarhei
Brenner, Günter
Eichmann, Ulrich
Korff Schmising, Clemens von
Beye, Martin
Eisebitt, Stefan
Type: Article
Abstract: Extending nonlinear spectroscopic techniques into the x-ray domain promises unique insight into photoexcited charge dynamics, which are of fundamental and applied interest. We report on the observation of a third-order nonlinear process in lithium fluoride (LiF) at a free-electron laser. Exploring the yield of four-wave mixing (FWM) in resonance with transitions to strongly localized core exciton states versus delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: Substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflective geometry–based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions, and can be easily scaled to shorter wavelengths at free-electron x-ray lasers.
Subject(s): hole colocalization
extreme ultraviolet
probing electron
nonlinear spectroscopic techniques
Issue Date: 20-May-2022
Date Available: 20-Jun-2022
Language Code: en
DDC Class: 530 Physik
Journal Title: Science Advances
Publisher: American Association for the Advancement of Science
Volume: 8
Issue: 20
Article Number: eabn5127
Publisher DOI: 10.1126/sciadv.abn5127
EISSN: 2375-2548
TU Affiliation(s): Fak. 2 Mathematik und Naturwissenschaften » Inst. Optik und Atomare Physik » FG Röntgenoptik und Nanometer-Optik
Appears in Collections:Technische Universität Berlin » Publications

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