Ultrafast X-ray Auger probing of photoexcited molecular dynamics
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Molecules can efficiently and selectively convert light energy into other degrees of freedom. Disentangling the underlying ultrafast motion of electrons and nuclei of the photoexcited molecule presents a challenge to current spectroscopic approaches. Here we explore the photoexcited dynamics of molecules by an interaction with an ultrafast X-ray pulse creating a highly localized core hole that decays via Auger emission. We discover that the Auger spectrum as a function of photoexcitation--X-ray-probe delay contains valuable information about the nuclear and electronic degrees of freedom from an element-specific point of view. For the nucleobase thymine, the oxygen Auger spectrum shifts towards high kinetic energies, resulting from a particular C-O bond stretch in the ππ* photoexcited state. A subsequent shift of the Auger spectrum towards lower kinetic energies displays the electronic relaxation of the initial photoexcited state within 200 fs. Ab-initio simulations reinforce our interpretation and indicate an electronic decay to the nπ* state.
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A longstanding controversy over the detailed photoprotection mechanisms of nucleobases was resolved through a combination of femtosecond Auger spectroscopy and time-resolved x-ray absorption.
“A longstanding controversy over the detailed photoprotection mechanisms of nucleobases was resolved through a combination of femtosecond Auger spectroscopy and time-resolved x-ray absorption [16].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [16]
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- Authors
- McFarland, B. K., Farrell, J. P., Miyabe, S., Tarantelli, F., Aguilar, A., Berrah, N., Bostedt, C., Bozek, J. D., Bucksbaum, P. H., Castagna, J. C., Coffee, R. N., Cryan, J. P., Fang, L., Feifel, R., Gaffney, K. J., Glownia, J. M., Martinez, T. J., Mucke, M., Murphy, B., Natan, A., Osipov, T., Petrović, V. S., Schorb, S., Schultz, T., Spector, L. S., Swiggers, M., Tenney, I., Wang, S., White, J. L., White, W., & Gühr, M.
- Affiliations
- SLAC National Accelerator Laboratory (US)
- University of Perugia (IT)
- Lawrence Berkeley National Laboratory (US)
- University of Connecticut (US)
- Western Michigan University (US)
- Uppsala University (SE)
- Corresponding author
- Gühr, M.
- ORCID
- Venue
- Nature Communications
- Published
- 2014-06-23
- Volume
- 5
- Issue
- 1
- Pages
- 4235-4235
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2035280333
- Cited by
- 161
- References
- 50
- Citations by year
- 2026: 2 · 2025: 6 · 2024: 8 · 2023: 11 · 2022: 14 · 2021: 10 · 2020: 13 · 2019: 9 · 2018: 20 · 2017: 17 · 2016: 22 · 2015: 24 · 2014: 5
- FWCI
- 11.28
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Licence
- Locations
- Nature Communications (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- KTH Publication Database DiVA (KTH Royal Institute of Technology) (submittedVersion, other-oa)
- RePEc: Research Papers in Economics (submittedVersion)
- Scholarworks@UNIST (Ulsan National Institute of Science and Technology) (submittedVersion)
- Funders
- U.S. Department of Energy (-AC02-05CH11231, Contract No. DE-AC02-05-CH11231, 05CH11231, No. DE-AC02-05-CH11231, DE AC02 05CH11231, DE-AC02-)
- Knut och Alice Wallenbergs Stiftelse
- Vetenskapsrådet
- Office of Science (No. DE-AC02- 05-CH11231, DEAC02–05CH11231, AC02-05CH11231, DE-AC02, Contract No. DE-AC02-05CH11231)
- Basic Energy Sciences (DE-AC02, Contract No. DE-AC02-05-CH11231, DE-AC02-05CH11231., No. DE-AC02-05-CH11231, AC02–05CH11231)
- Chemical Sciences, Geosciences, and Biosciences Division (DE-AC0205CH11231)
- SLAC National Accelerator Laboratory (DE-AC02-05-CH11231)
- 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
- X-ray pump-probe, core hole, thymine, ππ* excited states, electronic relaxation, nπ* states, NMR relaxation, ultrafast electron dynamics
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