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We demonstrate a new X-ray spectroscopy technique using four-photon interactions to probe electron dynamics at the atomic scale. This method offers unprecedented insights into ultrafast electronic processes in various materials.

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Area of Science:

  • Atomic and Molecular Physics
  • Ultrafast Spectroscopy
  • Quantum Electronics

Background:

  • Coherent nonlinear light-matter interactions with X-rays enable ultrafast spectroscopy at atomic resolution.
  • X-ray four-wave mixing offers insights into electronic state coupling, electron motion, and dynamics.
  • Current methods face limitations in achieving site and state selectivity for complex systems.

Purpose of the Study:

  • To demonstrate coherent, background-free four-photon interactions with core-shell electrons using X-ray pulses.
  • To explore X-ray four-wave mixing for atomic-scale multidimensional correlation spectroscopy.
  • To establish a foundation for studying localized electron dynamics with high resolution.

Main Methods:

  • Utilizing single broadband X-ray pulses from a free-electron laser.
  • Performing all-X-ray four-wave mixing measurements on gaseous neon.
  • Employing multicolour time-delayed X-ray pulse schemes.

Main Results:

  • Successfully demonstrated coherent, background-free four-photon interactions with core-shell electrons.
  • Observed X-ray four-wave mixing signals arising from doubly resonant nonlinear Raman processes.
  • Generated 2D spectral maps (photon-in/photon-out) for atomic-scale correlation spectroscopy.
  • Showcased the feasibility of ultrafast time-domain extensions using time-delayed pulses.

Conclusions:

  • The developed X-ray four-wave mixing technique provides atomic-scale insights into electron dynamics.
  • This methodology advances multidimensional correlation spectroscopy.
  • Potential applications include studying biomolecules, quantum materials, and advancing energy conversion and quantum technologies.