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Cited by 175Laser-Matter Interactions and ApplicationsX-ray Spectroscopy and Fluorescence AnalysisAtomic and Molecular Physics

The DOI matches its Crossref record; 32 of the 33 references it cites were found in a registry or an index.

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays

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Rudenko, A., Inhester, L., Hanasaki, K., Li, X., Robatjazi, S. J., Erk, B., Boll, R., Toyota, K., Hao, Y., Vendrell, O., Bomme, C., Savelyev, E., Rudek, B., Foucar, L., Southworth, S. H., Lehmann, C. S., Kraessig, B., Marchenko, T., Simon, M., Ueda, K., Ferguson, K. R., Bucher, M., Gorkhover, T., Carron, S., Alonso-Mori, R., Koglin, J. E., Correa, J., Williams, G. J., Boutet, S., Young, L., Bostedt, C., Son, S.-K., Santra, R., Rolles, D.·2017·Nature
DOI 10.1038/nature22373
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Abstract

X-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10 20 watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecular system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects-an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure-the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10 20 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.

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Authors
Rudenko, A., Inhester, L., Hanasaki, K., Li, X., Robatjazi, S. J., Erk, B., Boll, R., Toyota, K., Hao, Y., Vendrell, O., Bomme, C., Savelyev, E., Rudek, B., Foucar, L., Southworth, S. H., Lehmann, C. S., Kraessig, B., Marchenko, T., Simon, M., Ueda, K., Ferguson, K. R., Bucher, M., Gorkhover, T., Carron, S., Alonso-Mori, R., Koglin, J. E., Correa, J., Williams, G. J., Boutet, S., Young, L., Bostedt, C., Son, S.-K., Santra, R., & Rolles, D.
Affiliations
  • Kansas State University (US)
  • Deutsches Elektronen-Synchrotron DESY (DE)
  • Tohoku University (JP)
  • Aarhus University (DK)
  • Physikalisch-Technische Bundesanstalt (DE)
  • Max Planck Institute for Medical Research (DE)
  • Argonne National Laboratory (US)
  • Centre National de la Recherche Scientifique (FR)
  • SLAC National Accelerator Laboratory (US)
  • Brookhaven National Laboratory (US)
  • Northwestern University (US)
  • Universität Hamburg (DE)
Corresponding author
  • Rudenko, A.
  • Son, S.-K.
ORCID
Venue
Nature
Publisher
Springer Science and Business Media LLC
Published
2017-05-31
Volume
546
Issue
7656
Pages
129-132
ISSN
  • 0028-0836 (ISSN-L)
  • 1476-4687
DOI
10.1038/nature22373
OpenAlex
W2619312983
Cited by
175
References
33
Citations by year
2026: 12 · 2025: 12 · 2024: 9 · 2023: 20 · 2022: 22 · 2021: 19 · 2020: 30 · 2019: 24 · 2018: 23 · 2017: 4
FWCI
10.86
Type
journal article
Language
en
Open access
Licence
www.springer.com/tdm (tdm)
Locations
  • Nature (publishedVersion)
  • PubMed (publishedVersion)
  • K-State Research Exchange (Kansas State University) (submittedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
  • HAL (submittedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DESY Publication Database (PUBDB) (Deutsches Elektronen-Synchrotron) (submittedVersion)
  • Max Planck Digital Library (submittedVersion)
  • GoeScholar The Publication Server of the Georg-August-Universität Göttingen (Georg-August-Universität Göttingen) (submittedVersion, cc-by)
  • Scopus (Elsevier) (submittedVersion)
  • MPG.PuRe (Max Planck Society) (submittedVersion)
Funders
  • National Science Foundation (1430493, DE-AC02-76SF00515, DE-AC02–06CH11357, DE-SC0012704)
  • U.S. Department of Energy (DE‐ AC02‐06CH11357, DE‐FG02‐, 76SF00515, DE‐SC0012704, AC02‐06CH11357, DE–AC02–76SF00515, AC02‐76SF00515, SC0012704., 06CH11357, FG02-86ER13491, DE-AC02-, DEFG0286ER13491)
  • Helmholtz-Gemeinschaft
  • Deutsche Forschungsgemeinschaft (DE-AC02-06CH11357, DE-AC02-76SF00515)
  • Volkswagen Foundation
  • Ministry of Education, Culture, Sports, Science and Technology (DE-AC02-06CH11357)
  • Hamburg Centre for Ultrafast Imaging
  • Office of Science (AC02-76SF00515, AC02‐06CH11357, DEFG0286ER13491, DE-SC-0012704, DE-AC02-76SF0051 5, DE-AC02, FG02-86ER13491, 06CH11357, SC0012704, 76SF00515, DE-AC02-06CH11357)
  • Basic Energy Sciences (DE-AC02, DE- SC0012704, FG02-86ER13491, DEFG02-86ER13491, DE-AC- 02-06CH11357, AC02‐06CH11357, DE-FG02, 76SF00515, SC0012704, AC02-76SF00515, 06CH11357, DE-AC-02-76SF00515)
  • Chemical Sciences, Geosciences, and Biosciences Division (DE-FG02- 86ER13491, DE-FG02, SC0012704, DE-SC0012704, DE-AC-0206CH11357, DE-AC02-76SF00515)
  • Office of Experimental Program to Stimulate Competitive Research (1430493, DE-AC02-06CH11357, IIA-1430493)
  • Argonne National Laboratory (DE- AC02-06-CH11357, DE-AC02, AC02–06CH11357, DE-SC0012704, 06CH11357, DE-AC02-76SF00515)
  • SLAC National Accelerator Laboratory (DEAC02−76SF00515, AC02‐76SF00515, DE-AC02-06CH11357)
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 › Atomic and Molecular Physics, and Optics › Atomic and Molecular Physics
Keywords
polyatomic molecules, X-ray free-electron laser, ultrafast charge transfer, radiation damage, serial femtosecond crystallography, phasing, multiphoton absorption, femtosecond dynamics
MeSH terms
Crystallography, Electrons, Iodine, Kinetics, Lasers, Protein Conformation, Proteins, Time Factors, X-Rays, Photons, Static Electricity

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