Ultrafast X-ray-induced dephasing of valence electrons
Authors: J. Vonka (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), B. Pedrini (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), J. Ravnik (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), A. Steppke (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), E. Prat (PSI Center for Accelerator Science and Engineering, Paul Scherrer Institute, Villigen PSI, Switzerland), S. Reiche (PSI Center for Accelerator Science and Engineering, Paul Scherrer Institute, Villigen PSI, Switzerland), D. G. Mazzone (PSI Center for Neutron and Muon Sciences, Paul Scherrer Institute, Villigen PSI, Switzerland), P. Anand (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), S. Allenspach (PSI Center for Neutron and Muon Sciences, Paul Scherrer Institute, Villigen PSI, Switzerland), Y. Ekinci (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), U. Staub (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), S. -W. Huang (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), M. Sander (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), R. Mankowsky (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), H. T. Lemke (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), G. Aeppli (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland), S. Gerber (PSI Center for Photon Science, Paul Scherrer Institute, Villigen PSI, Switzerland)
Abstract
Diffract-before-destroy schemes for atomic-scale electron mapping assume that ultrashort X-ray pulses outrun radiation damage. Although atomic cores move over tens of femtoseconds, outer electrons respond much faster, compromising their locations. We test this limit in elemental silicon using broadband, energy-chirped X-ray pulses to encode time with few-femtosecond resolution. Comparing valence-sensitive structurally forbidden reflections with simultaneously measured core-dominated Bragg peaks reveals valence-bond dephasing on sub-20-fs timescales even at pulse energies where direct ionization effects are negligible. Our findings demonstrate that crystallography where outer electrons contribute substantially to Bragg peaks requires pulses shorter than today's standard $\sim50\,fs$ standard. They also establish a path to disentangle valence electron and lattice contributions to order and dynamics with hard X-rays, enabling studies across molecular biology, quantum matter and devices.
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Electronic Damage Suppression in X-ray Diffraction with Attosecond X-ray PulsesV. Lipp, Ichiro Inoue, B. Ziaja · 2026 · cited 1 time · Not summarized yet
Electronic Damage Suppression proposes attosecond hard X-ray pulses to limit electronic excitation during diffraction, while this paper measures valence-bond dephasing in silicon.
Abstract
So far, the focus of state-of-the-art structure determination using x-ray free-electron laser (XFEL) pulses has been on macromolecular crystallography. This approach has achieved remarkable success in solving the structure of microcrystals smaller than a few micrometres, which are difficult to investigate using conventional synchrotron sources. However, successful applications of XFELs to inorganic and small-molecule crystallography have been limited due to rapid electron excitation in these samples. This same issue has also prevented the use of XFELs in charge-density studies of solids. In this study, we propose using hard x-ray pulses with an attosecond duration for x-ray imaging of charge…
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Imaging of femtosecond bond breaking and charge dynamics in ultracharged peptides.Ibrahim Eliah Dawod, N. Tîmneanu, A. Mancuso et al. · 2021 · Physical Chemistry, Chemical Physics - PCCP · cited 4 times · Not summarized yet
Imaging ultracharged peptides examines femtosecond bond breaking and charge dynamics under X-ray irradiation, rather than valence-sensitive diffraction in silicon.
Abstract
X-ray free-electrons lasers have revolutionized the method of imaging biological macromolecules such as proteins, viruses and cells by opening the door to structural determination of both single particles and crystals at room temperature. By utilizing high intensity X-ray pulses on femtosecond timescales, the effects of radiation damage can be reduced. Achieving high resolution structures will likely require knowledge of how radiation damage affects the structure on an atomic scale, since the experimentally obtained electron densities will be reconstructed in the presence of radiation damage. Detailed understanding of the expected damage scenarios provides further information, in addition to…
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Structural dynamics in proteins induced by and probed with X-ray free-electron laser pulsesK. Nass, A. Gorel, Malik M. Abdullah et al. · 2020 · Nature Communications · cited 83 times · Not summarized yet
Structural dynamics in proteins measures XFEL-induced atomic motion in protein nanocrystals, whereas this paper probes faster valence-electron dephasing in silicon.
Abstract
X-ray free-electron lasers (XFELs) enable crystallographic structure determination beyond the limitations imposed upon synchrotron measurements by radiation damage. The need for very short XFEL pulses is relieved through gating of Bragg diffraction by loss of crystalline order as damage progresses, but not if ionization events are spatially non-uniform due to underlying elemental distributions, as in biological samples. Indeed, correlated movements of iron and sulfur ions were observed in XFEL-irradiated ferredoxin microcrystals using unusually long pulses of 80 fs. Here, we report a femtosecond time-resolved X-ray pump/X-ray probe experiment on protein nanocrystals. We observe changes in th…
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Diffraction before destructionH. Chapman, C. Caleman, N. Tîmneanu · 2014 · Philosophical Transactions of the Royal Society B: Biological Sciences · cited 222 times · Not summarized yet
Diffraction before destruction describes collecting diffraction before XFEL pulses destroy samples, the principle this paper tests for valence-electron states.
Abstract
X-ray free-electron lasers have opened up the possibility of structure determination of protein crystals at room temperature, free of radiation damage. The femtosecond-duration pulses of these sources enable diffraction signals to be collected from samples at doses of 1000 MGy or higher. The sample is vaporized by the intense pulse, but not before the scattering that gives rise to the diffraction pattern takes place. Consequently, only a single flash diffraction pattern can be recorded from a crystal, giving rise to the method of serial crystallography where tens of thousands of patterns are collected from individual crystals that flow across the beam and the patterns are indexed and aggrega…
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Radiation damage in protein serial femtosecond crystallography using an x-ray free-electron laserL. Lomb, T. Barends, S. Kassemeyer et al. · 2011 · Physical review. B, Condensed matter and materials physics · cited 163 times · Not summarized yet
Radiation damage in protein serial femtosecond crystallography measures pulse-length and fluence effects on lysozyme diffraction, rather than valence-electron dephasing.
Abstract
X-ray free-electron lasers deliver intense femtosecond pulses that promise to yield high resolution diffraction data of nanocrystals before the destruction of the sample by radiation damage. Diffraction intensities of lysozyme nanocrystals collected at the Linac Coherent Light Source using 2 keV photons were used for structure determination by molecular replacement and analyzed for radiation damage as a function of pulse length and fluence. Signatures of radiation damage are observed for pulses as short as 70 fs. Parametric scaling used in conventional crystallography does not account for the observed effects.
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Interplay of thermal and nonthermal effects in x-ray-induced ultrafast meltingI. Inoue, V. Tkachenko, Y. Kubota et al. · 2023 · Physical review B · cited 5 times · Not summarized yet
Interplay of thermal and nonthermal effects investigates ultrafast X-ray-induced changes in silicon, but tracks melting and atomic disorder rather than valence-bond dephasing.
Abstract
X-ray laser-induced structural changes in silicon undergoing femtosecond melting have been investigated by using an x-ray pump-x-ray probe technique. The experimental results for different initial sample temperatures reveal that the onset time and the speed of the atomic disordering are independent of the initial temperature, suggesting that equilibrium atomic motion in the initial state does not play a pivotal role in the x-ray-induced ultrafast melting. By comparing the observed time-dependence of the atomic disordering and the dedicated theoretical simulations, we interpret that the energy transfer from the excited electrons to ions via electron-ion coupling (thermal effect) as well as a …
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Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron LaserZhao-Heng Guo, T. Driver, S. Beauvarlet et al. · 2024 · cited 37 times · Not summarized yet
Experimental Demonstration generates and controls sub-femtosecond XFEL pulse pairs for spectroscopy, a pulse capability relevant to resolving electronic dynamics.
Abstract
Pump-probe experiments with sub-femtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of sub-femtosecond pulse pairs from a two-colour X-ray free-electron laser (XFEL). By measuring the delay between the two pulses with an angular streaking diagnostic, we characterise the group velocity of the XFEL and demonstrate control of the pulse delay down to 270 as. We demonstrate the application of this technique to a pump-probe measurement in core-excited para-aminophenol. These results demonstrate the ability to perform pump-probe experiments with sub-femtosecond resolution and atomic site specificity.
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Femtosecond Three-Dimensional Imaging of Single-Protein with Hard X-ray Laser.P. L. Xavier, Andrew J. Morgan, J. Bielecki et al. · 2026 · arXiv.org · preprint, not peer reviewed · Not summarized yet
Femtosecond Three-Dimensional Imaging develops hard-X-ray imaging of single proteins, addressing radiation-sensitive structural imaging rather than electronic damage in silicon.
Abstract
The extremely intense pulses of X-ray free-electron lasers (XFELs) have enabled imaging of radiation-sensitive samples, such as macromolecular microcrystals, beyond radiation damage limits. These sources have the potential to deliver biomolecular single-particle imaging, similar to cryo-electron microscopy but without the need for cryo-fixation and with temporal resolution from femtoseconds to milliseconds. While this possibility was recognized before XFELs were built, the biological single-particle imaging work-flow has previously only been demonstrated on large virus particles. Based on decades of improvements in X-ray beam focusing, particle delivery, diffraction detection, and advanced a…
Prior work it builds on
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Millijoule Femtosecond X-Ray Pulses from an Efficient Fresh-Slice Multistage Free-Electron Laser.Guang-Lei Wang, P. Dijkstal, S. Reiche et al. · 2024 · Physical Review Letters · cited 12 times · Not summarized yet
Millijoule Femtosecond X-Ray Pulses demonstrates an XFEL source producing intense, short X-ray pulses, a generic capability for ultrafast X-ray experiments.
Abstract
We present the generation of x-ray pulses with average pulse energies up to one millijoule and rms pulse durations down to the femtosecond level. We have produced these intense and short pulses by employing the fresh-slice multistage amplification scheme with a transversely tilted electron beam in a free-electron laser. In this scheme, a short pulse is produced in the first stage and later amplified by fresh parts of the electron bunch in up to a total of four stages of amplification. Our implementation is efficient, since practically the full electron beam contributes to produce the x-ray pulse. Our implementation is also compact, utilizing only 32 m of undulator. The demonstration was done…
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Megahertz single-particle imaging at the European XFELE. Sobolev, S. Zolotarev, K. Giewekemeyer et al. · 2019 · Communications Physics · cited 73 times · Not summarized yet
Megahertz single-particle imaging concerns high-rate XFEL measurements of biological particles, not the electronic response of silicon to individual pulses.
Abstract
The emergence of high repetition-rate X-ray free-electron lasers (XFELs) powered by superconducting accelerator technology enables the measurement of significantly more experimental data per day than was previously possible. The European XFEL is expected to provide 27,000 pulses per second, over two orders of magnitude more than any other XFEL. The increased pulse rate is a key enabling factor for single-particle X-ray diffractive imaging, which relies on averaging the weak diffraction signal from single biological particles. Taking full advantage of this new capability requires that all experimental steps, from sample preparation and delivery to the acquisition of diffraction patterns, are …
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Terawatt-attosecond hard X-ray free-electron laser at high repetition rateJia-Wei Yan, Weilun Qin, Ye Chen et al. · 2024 · Nature Photonics · cited 70 times · Not summarized yet
Terawatt-attosecond hard X-ray free-electron laser demonstrates high-power attosecond pulses, a source capability for probing electronic dynamics.
Abstract
Ångstrom and attosecond are the fundamental spatiotemporal scales for electron dynamics in various materials. Although attosecond pulses with wavelengths comparable to the atomic scales are expected to be a key tool in advancing attosecond science, producing high-power hard X-ray attosecond pulses at ångstrom wavelengths remains a formidable challenge. Here, we report the generation of terawatt-scale attosecond hard X-ray pulses using a free-electron laser in a special operation mode. We achieved 9 keV single-spike X-ray pulses with a mean pulse energy of around 180 μJ, exceeding previous reports by more than an order of magnitude, and an estimated average pulse duration of 200 as at full-wi…
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Delayed Onset and Directionality of X-Ray-Induced Atomic Displacements Observed on Subatomic Length Scales.I. Inoue, V. Tkachenko, K. Kapcia et al. · 2021 · Physical Review Letters · cited 12 times · Not summarized yet
Delayed Onset and Directionality measures X-ray-induced atomic displacements in alumina, while this paper measures valence-electron dephasing in silicon.
Abstract
Transient structural changes of Al_{2}O_{3} on subatomic length scales following irradiation with an intense x-ray laser pulse (photon energy: 8.70 keV; pulse duration: 6 fs; fluence: 8×10^{2} J/cm^{2}) have been investigated by using an x-ray pump x-ray probe technique. The measurement reveals that aluminum and oxygen atoms remain in their original positions by ∼20 fs after the intensity maximum of the pump pulse, followed by directional atomic displacements at the fixed unit cell parameters. By comparing the experimental results and theoretical simulations, we interpret that electron excitation and relaxation triggered by the pump pulse modify the potential energy surface and drives the di…
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Serial Femtosecond CrystallographyH. Chapman · 2015 · Synchrotron Radiation News · cited 50 times · Not summarized yet
Serial Femtosecond Crystallography presents the XFEL diffraction approach used to collect structural information before radiation damage destroys a sample.
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