Femtosecond response of polyatomic molecules to ultra-intense hard X-rays
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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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At extreme x-ray intensities exceeding 10^19 W cm^-2, ionization of a small molecule can be significantly enhanced via recurrent charge redistribution, resulting in emission of more than 50 electrons within few tens of fs.
“In particular, it has been shown that at extreme x-ray intensities (exceeding 10 19 W cm -2 ), the ionization of a small molecule can be significantly enhanced via a recurrent charge redistribution resulting in the emission of more than 50 electrons within few tens of fs [87].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [87]
Recent theoretical efforts have yielded a quantitative understanding of ionization and fragmentation dynamics for CH3I molecules under extremely intense hard x-ray light.
“Nevertheless, recent theoretical efforts have yielded a quantitative understanding of ionization and fragmentation dynamics for CH 3 I molecules under extremely intense hard x-ray light [87].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [87]
By eliminating a key shortcoming of XMDYN, it was possible, utilizing XMOLECULE, to identify a new ionization enhancement mechanism that involves ultrafast electron redistribution through chemical bonds [87].
“By eliminating a key shortcoming of XMDYN, it was possible, utilizing XMOLECULE, to identify a new ionization enhancement mechanism that involves ultrafast electron redistribution through chemical bonds [87].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [87]
A first step towards overcoming the molecular electronic-structure challenge in high-intensity x-ray physics is XMOLECULE [87].
“A first step towards overcoming the molecular electronicstructure challenge in high-intensity x-ray physics is XMOLECULE [87].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [87]
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Self-citationObserving pre-edge K -shell resonances in Kr, Xe, and XeF2
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Multiphoton Ionization Reduction of Atoms in Two-Color Femtosecond Laser Fields
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Ultraviolet Pump–Probe Photodissociation Spectroscopy of Electron-Rotation Coupling in Diatomics
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Self-citationMegahertz-compatible angular streaking with few-femtosecond resolution at x-ray free-electron lasers
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A Reaction Microscope for AMO Science at Shanghai Soft X-ray Free-Electron Laser Facility
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Self-citationSimple model for sequential multiphoton ionization by ultraintense x rays
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Self-citationAttosecond pump–attosecond probe spectroscopy of Auger decay
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State-resolved ionization dynamics of a neon atom induced by x-ray free-electron-laser pulses
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Self-citationLaser-induced deformation of triatomic molecules: Influence on tunnel ionization
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Convergent-beam attosecond x-ray crystallography
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Coulomb explosion of CD3I induced by single photon deep inner-shell ionisation
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Self-citationStatistical analysis of correlations in the x-ray induced Coulomb explosion of iodopyridine
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Self-citationResonance-enhanced x-ray multiple ionization of a polyatomic molecule
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Self-citationLaser-Induced Alignment of Molecules in Helium Nanodroplets
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Highly efficient nanoscale X-ray sources
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Online single-shot characterization of ultrafast pulses from high-gain free-electron lasers
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Mapping ultrafast ionization of atoms and clusters with terahertz-streaking delay
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Photo-ionization and fragmentation of Sc3N@C80 following excitation above the Sc K-edge
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Self-citationMeasuring Charge Distribution of Molecular Cations by an Atomic Coulomb Probe Microscope
Yu, X., Hu, X., Zhou, J., Zhang, X., Zhao, X., Jia, S., Xue, X., Ren, D., Li, X., Wu, Y., et al. (2022) · Chinese Physics Letters · doi:10.1088/0256-307x/39/11/113301 · Cited by 6 · see citing works
Self-citationThe contribution of Compton ionization to ultrafast x-ray scattering
Ziems, K. M., Simmermacher, M., Gräfe, S., & Kirrander, A. (2023) · The Journal of Chemical Physics · doi:10.1063/5.0156363 · Cited by 6 · see citing works
Femtosecond laser produced periodic plasma in a colloidal crystal probed by XFEL radiation
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Self-citation
- 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
- Published
- 2017-05-31
- Volume
- 546
- Issue
- 7656
- Pages
- 129-132
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- 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
- green
- hdl.handle.net
- 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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