期刊
SCIENCE ADVANCES
卷 8, 期 20, 页码 -出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abn5127
关键词
-
资金
- Helmholtz foundation [VH-NG-1105]
Extending nonlinear spectroscopic techniques into the x-ray domain allows for unique insights into photoexcited charge dynamics. We have observed a third-order nonlinear process in lithium fluoride (LiF) and found that resonant four-wave mixing (FWM) can be used as a sensitive probe for charge localization.
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.
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