Photon-recoil imaging: Expanding the view of nonlinear x-ray physics

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Science  25 Sep 2020:
Vol. 369, Issue 6511, pp. 1630-1633
DOI: 10.1126/science.abc2622

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Nonlinear x-ray spectroscopy

The extension of nonlinear optics to the x-ray spectral domain is a promising direction in the development of x-ray spectroscopy. Although theoretical concepts of nonlinear x-ray spectroscopy were developed decades ago, scientists still struggle to implement them because of the elusive nature of nonlinear effects. Eichmann et al. now present atomic momentum spectroscopy (AMS), which is based on the detection of the scattered atom after momentum transfer from x-ray photons (see the Perspective by Pfeifer). The authors show how AMS can observe stimulated x-ray Raman scattering signals at the neon K edge on a single-atom level and distinguish them from other competing processes. These results pave the way for future nonlinear x-ray spectroscopy methods for the study of x-ray–matter interactions.

Science, this issue p. 1630; see also p. 1568


Addressing the ultrafast coherent evolution of electronic wave functions has long been a goal of nonlinear x-ray physics. A first step toward this goal is the investigation of stimulated x-ray Raman scattering (SXRS) using intense pulses from an x-ray free-electron laser. Earlier SXRS experiments relied on signal amplification during pulse propagation through dense resonant media. By contrast, our method reveals the fundamental process in which photons from the primary radiation source directly interact with a single atom. We introduce an experimental protocol in which scattered neutral atoms rather than scattered photons are detected. We present SXRS measurements at the neon K edge and a quantitative theoretical analysis. The method should become a powerful tool in the exploration of nonlinear x-ray physics.

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