Li, Kai
; Ott, Christian
; Agaker, Marcus
; ... - Nature
Propagation of intense x-ray pulses through dense media has led to the observation of striking phenomena, such as atomic x-ray lasing [1, 2], self-induced transparency [3] and stimulated x-ray Raman scattering (SXRS) [4]. SXRS has been long envisioned as means to launch and probe valence-electron wavepackets and as a building block for nonlinear x-ray spectroscopies [5, 6]. However, experimental observations of SXRS to date [4, 7, 8] have not provided spectroscopic information and theoretical modeling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, i.e. detection of valence-excited states in neon with a near Fourier-limited
more » joint energy-time resolution of 0.1 eV-40 fs. Instead of requiring intense phase-controlled attosecond pulses, we employed a novel covariance analysis between statistically spiky broadband incident x-ray and scattered x-ray Raman pulses. Using 18000 single shots we not only beat the incident (∼ 8 eV) bandwidth but also the ∼ 0.2 eV instrumental energy resolution, thus creating super-resolution conditions, in analogy to super-resolved fluorescence microscopy [9]. Our experimental results, supported by ab initio propagation simulations, reveal the competition between lasing in the ion and stimulated Raman scattering in the neutral. We demonstrate enhanced signal collection efficiency and broad excitation window, surpassing spontaneous Raman efficiencies by orders of magnitude. We anticipate our approach as the starting point for further application of stochastic stimulated x-ray Raman spectroscopies to detect passage through the ubiquitous conical intersections encountered in photochemistry, enabling one to track elementary events that determine chemical outcomes [10].« less