Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning

Free-electron lasers providing ultra-short high-brightness pulses of X-ray radiation have great potential for a wide impact on science, and are a critical element for unravelling the structural dynamics of matter. To fully harness this potential, we must accurately know the X-ray properties: intensity, spectrum and temporal profile. Owing to the inherent fluctuations in free-electron lasers, this mandates a full characterization of the properties for each and every pulse. While diagnostics of these properties exist, they are often invasive and many cannot operate at a high-repetition rate. Here, we present a technique for circumventing this limitation. Employing a machine learning strategy, we can accurately predict X-ray properties for every shot using only parameters that are easily recorded at high-repetition rate, by training a model on a small set of fully diagnosed pulses. This opens the door to fully realizing the promise of next-generation high-repetition rate X-ray lasers

Resonant inelastic x-ray scattering at the N2 π*-resonance: Lifetime-vibrational interference, radiative electron rearrangement, and wave-function imaging

Resonant inelastic x-ray scattering spectra excited at the pi*-resonance of the nitrogen molecule are presented. Well-resolved vibrational excitations in the electronic ground state, and in the 3 sigma g(-1 )1 pi(1)(g) a(1) Pi(g) state are observed. The spectra are analyzed within the Kramers-Heisenberg formalism, and the importance of lifetime-vibrational interference effects is highlighted. In addition, strongly dissociative multiply excited final states populated in radiative electron rearrangement are found in the valence ionization continua. The vibrational wave functions of the core-excited state are imaged on the strongly dissociative final state potentials

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

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

Magnetic circular dichroism in the dd excitation in the van der Waals magnet CrI3 probed by resonant inelastic x-ray scattering

We report on a combined experimental and theoretical study on CrI3 single crystals by employing the polarization dependence of resonant inelastic x-ray scattering (RIXS). Our investigations reveal multiple Cr 3d orbital splitting (dd excitations) as well as magnetic dichroism (MD) in the RIXS spectra. The dd excitation energies are similar on the two sides of the ferromagnetic transition temperature, T-C similar to 61 K, although MD in RIXS is predominant at 0.4 T magnetic field below TC. This demonstrates that the ferromagnetic superexchange interaction that is responsible for the interatomic exchange field is vanishingly small compared with the local exchange field that comes from exchange and correlation interaction among the interacting Cr 3d orbitals. The recorded RIXS spectra reported here reveal clearly resolved Cr 3d intraorbital dd excitations that represent transitions between electronic levels that are heavily influenced by dynamic correlations and multiconfiguration effects. Our calculations taking into account the Cr 3d hybridization with the ligand valence states and the full multiplet structure due to intra-atomic and crystal field interactions in Oh and D3d symmetry clearly reproduced the dichroic trend in experimental RIXS spectra