X-ray Raman scattering: a building block for nonlinear spectroscopy

Ultraintense X-ray free-electron laser pulses of attosecond duration can enable new nonlinear X-ray spectroscopic techniques to observe coherent electronic motion. The simplest nonlinear X-ray spectroscopic concept is based on stimulated electronic X-ray Raman scattering. We present a snapshot of recent experimental achievements, paving the way towards the goal of realizing nonlinear X-ray spectroscopy. In particular, we review the first proof-of-principle experiments, demonstrating stimulated X-ray emission and scattering in atomic gases in the soft X-ray regime and first results of stimulated hard X-ray emission spectroscopy on transition metal complexes. We critically asses the challenges that have to be overcome for future successful implementation of nonlinear coherent X-ray Raman spectroscopy. This article is part of the theme issue 'Measurement of ultrafast electronic and structural dynamics with X-rays'.