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PreprintarXiv licencearXiv

Ultrafast X-ray-induced dephasing of valence electrons

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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 ∼50 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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BibTeX
@misc{vonka2026ultrafast,
  title = {{Ultrafast X-ray-induced dephasing of valence electrons}},
  author = {J. Vonka and B. Pedrini and J. Ravnik and A. Steppke and E. Prat and S. Reiche and D. G. Mazzone and P. Anand and S. Allenspach and Y. Ekinci and U. Staub and S. -W. Huang and M. Sander and R. Mankowsky and H. T. Lemke and G. Aeppli and S. Gerber},
  howpublished = {arXiv},
  year = {2026},
  month = nov,
  doi = {10.48550/arxiv.2611.03635},
  eprint = {2611.03635},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2611.03635},
}
RIS
TY  - UNPB
TI  - Ultrafast X-ray-induced dephasing of valence electrons
AU  - J. Vonka
AU  - B. Pedrini
AU  - J. Ravnik
AU  - A. Steppke
AU  - E. Prat
AU  - S. Reiche
AU  - D. G. Mazzone
AU  - P. Anand
AU  - S. Allenspach
AU  - Y. Ekinci
AU  - U. Staub
AU  - S. -W. Huang
AU  - M. Sander
AU  - R. Mankowsky
AU  - H. T. Lemke
AU  - G. Aeppli
AU  - S. Gerber
PY  - 2026
DA  - 2026/11/02
PB  - arXiv
DO  - 10.48550/arxiv.2611.03635
UR  - https://arxiv.org/abs/2611.03635
AB  - 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 ∼50 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.
ER  -