期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 108, 期 41, 页码 16912-16915出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1111380108
关键词
multi-photon ionization; ultrafast; two-photon spectroscopy
资金
- US Department of Energy, Office of Science, Basic Energy Science, Chemical, Geosciences, and Biological Divisions
- Ministry for Infrastucture, Universities and Research, Italy [FIRB-RBAP045JF2, FIRB-RBAP06AWK3]
- Japan Ministry of Education, Culture, Sports, Science and Technology
- Japan Science and Technology Agency
- Turku University Foundation
- Swedish Research Council (VR)
- Grants-in-Aid for Scientific Research [23750029, 23550017, 21350014, 21350019] Funding Source: KAKEN
Theory predicts that double-core-hole (DCH) spectroscopy can provide a new powerful means of differentiating between similar chemical systems with a sensitivity not hitherto possible. Although DCH ionization on a single site in molecules was recently measured with double-and single-photon absorption, double-core holes with single vacancies on two different sites, allowing unambiguous chemical analysis, have remained elusive. Here we report that direct observation of double-core holes with single vacancies on two different sites produced via sequential two-photon absorption, using short, intense X-ray pulses from the Linac Coherent Light Source free-electron laser and compare it with theoretical modeling. The observation of DCH states, which exhibit a unique signature, and agreement with theory proves the feasibility of the method. Our findings exploit the ultrashort pulse duration of the free-electron laser to eject two core electrons on a time scale comparable to that of Auger decay and demonstrate possible future X-ray control of physical inner-shell processes.
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