Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics
Open accessAbstract
New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site. Two-color X-ray pulses with controlled time delay allow exciting one site of a molecule and then probing a different site of the same molecule with femtosecond resolution. Here, the authors use this hetero-site pump-probe technique to study charge redistribution and dissociation of the xenon difluoride molecule.
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Optical light pulses can excite a nanoparticle as a whole, and x-ray pulses can be used to induce localized, element-specific excitations.
“Optical light pulses can excite the nanoparticle as a whole and x-ray pulses can be used to induce localized, element-specific excitations [101].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [101]
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Roadmap of ultrafast x-ray atomic and molecular physics
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Self-citation
- Authors
- Picón, A., Lehmann, C. S., Bostedt, C., Rudenko, A., Marinelli, A., Osipov, T., Rolles, D., Berrah, N., Bomme, C., Bucher, M., Doumy, G., Erk, B., Ferguson, K. R., Gorkhover, T., Ho, P. J., Kanter, E. P., Krässig, B., Krzywinski, J., Lutman, A. A., March, A. M., Moonshiram, D., Ray, D., Young, L., Pratt, S. T., & Southworth, S. H.
- Affiliations
- Argonne National Laboratory (US)
- Northwestern University (US)
- Kansas State University (US)
- SLAC National Accelerator Laboratory (US)
- University of Connecticut (US)
- Deutsches Elektronen-Synchrotron DESY (DE)
- Lawrence Berkeley National Laboratory (US)
- Corresponding author
- Picón, A.
- ORCID
- Venue
- Nature Communications
- Published
- 2016-05-23
- Volume
- 7
- Issue
- 1
- Pages
- 11652-11652
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC4879250
- OpenAlex
- W2403765023
- Cited by
- 88
- References
- 31
- Citations by year
- 2026: 3 · 2025: 3 · 2024: 8 · 2023: 6 · 2022: 9 · 2021: 11 · 2020: 8 · 2019: 6 · 2018: 16 · 2017: 13 · 2016: 4
- FWCI
- 6.15
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Licence
- Locations
- Nature Communications (publishedVersion, cc-by-nc-nd)
- Europe PMC (PubMed Central) (publishedVersion, cc-by-nc-nd)
- PubMed Central (publishedVersion, cc-by-nc-nd)
- PubMed (publishedVersion)
- K-State Research Exchange (Kansas State University) (submittedVersion, cc-by-nc-nd)
- MPG.PuRe (Max Planck Society) (submittedVersion, cc-by-nc-nd)
- RePEc: Research Papers in Economics (submittedVersion)
- Desy publication database (The Deutsches Elektronen-Synchrotron) (submittedVersion, other-oa)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- GoeScholar The Publication Server of the Georg-August-Universität Göttingen (Georg-August-Universität Göttingen) (submittedVersion, cc-by)
- DESY Publication Database (PUBDB) (Deutsches Elektronen-Synchrotron)
- Funders
- U.S. Department of Energy (DE‐ AC02‐06CH11357, DE‐FG02‐, 76SF00515, AC02‐06CH11357, DE–AC02–76SF00515, DESC0012376, AC02‐76SF00515, No. DE-AC02–76SF00515, 06CH11357, FG02-86ER13491, Contract No. DE-AC02-76SF00515, DE-AC02-, DEFG0286ER13491)
- Helmholtz-Gemeinschaft
- Volkswagen Foundation
- Office of Science (AC02-76SF00515, DESC0012376, AC02‐06CH11357, DEFG0286ER13491, DE-AC02-76SF0051 5, DE-AC02, FG02-86ER13491, 06CH11357, 76SF00515, DE-AC02-06CH11357)
- Basic Energy Sciences (DE-AC02, FG02-86ER13491, DEFG02-86ER13491, DE-SC0012376, DE-AC- 02-06CH11357, AC02‐06CH11357, DE-FG02, 76SF00515, Contract No. DE-AC02-76SF00515, AC02-76SF00515, 06CH11357, DE-AC-02-76SF00515)
- Chemical Sciences, Geosciences, and Biosciences Division (DE-FG02- 86ER13491, DE-FG02, DE_SC0012376, DE-AC-0206CH11357, DE-AC02-76SF00515)
- Argonne National Laboratory (DE- AC02-06-CH11357, DE-AC02, AC02–06CH11357, 06CH11357, DE-AC02-76SF00515)
- SLAC National Accelerator Laboratory (DEAC02−76SF00515, AC02‐76SF00515, DE-AC02-06CH11357, Contract No. DE-AC02-76SF00515)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
- Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
- Keywords
- charge redistribution, molecular dissociation, X-ray absorption, X-ray free-electron laser
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