Time-resolved RIXS experiment with pulse-by-pulse parallel readout data collection using X-ray free electron laser.

Time-resolved resonant inelastic X-ray scattering (RIXS) is one of the developing techniques enabled by the advent of X-ray free electron laser (FEL). It is important to evaluate how the FEL jitter, which is inherent in the self-amplified spontaneous emission process, influences the RIXS measurement. Here, we use a microchannel plate (MCP) based Timepix soft X-ray detector to conduct a time-resolved RIXS measurement at the Ti L3-edge on a charge-density-wave material TiSe2. The fast parallel Timepix readout and single photon sensitivity enable pulse-by-pulse data acquisition and analysis. Due to the FEL jitter, low detection efficiency of spectrometer, and low quantum yield of RIXS process, we find that less than 2% of the X-ray FEL pulses produce signals, preventing acquiring sufficient data statistics while maintaining temporal and energy resolution in this measurement. These limitations can be mitigated by using future X-ray FELs with high repetition rates, approaching MHz such as the European XFEL in Germany and LCLS-II in the USA, as well as by utilizing advanced detectors, such as the prototype used in this study

Measurements of the K-shell opacity of a solid-density magnesium plasma heated by an X-ray free electron laser

We present measurements of the spectrally-resolved X-rays emitted from solid-density magnesium targets of varying sub-μm thicknesses isochorically heated by an X-ray laser. The data exhibit a largely thickness-independent source function, allowing the extraction of a measure of the opacity to K-shell X-rays within well-defined regimes of electron density and temperature, extremely close to local thermodynamic equilibrium (LTE) conditions. The deduced opacities at the peak of the K-α transitions of the ions are consistent with those predicted by detailed atomic-kinetics calculations

Measurements of the K-shell opacity of a solid-density magnesium plasma heated by an X-ray free electron laser

We present measurements of the spectrally-resolved X-rays emitted from solid-density magnesium targets of varying sub-μm thicknesses isochorically heated by an X-ray laser. The data exhibit a largely thickness-independent source function, allowing the extraction of a measure of the opacity to K-shell X-rays within well-defined regimes of electron density and temperature, extremely close to local thermodynamic equilibrium (LTE) conditions. The deduced opacities at the peak of the K-α transitions of the ions are consistent with those predicted by detailed atomic-kinetics calculations

Ultrafast dynamics of localized magnetic moments in the unconventional Mott insulator Sr2IrO4.

We report a time-resolved study of the ultrafast dynamics of the magnetic moments formed by the [Formula: see text] states in Sr2IrO4 by directly probing the localized iridium 5d magnetic state through resonant x-ray diffraction. Using optical pump-hard x-ray probe measurements, two relaxation time scales were determined: a fast fluence-independent relaxation is found to take place on a time scale of 1.5 ps, followed by a slower relaxation on a time scale of 500 ps-1.5 ns

Nanosecond X-Ray Photon Correlation Spectroscopy on Magnetic Skyrmions.

We report an x-ray photon correlation spectroscopy method that exploits the recent development of the two-pulse mode at the Linac Coherent Light Source. By using coherent resonant x-ray magnetic scattering, we studied spontaneous fluctuations on nanosecond time scales in thin films of multilayered Fe/Gd that exhibit ordered stripe and Skyrmion lattice phases. The correlation time of the fluctuations was found to differ between the Skyrmion phase and near the stripe-Skyrmion boundary. This technique will enable a significant new area of research on the study of equilibrium fluctuations in condensed matter

Measurements of continuum lowering in solid-density plasmas created from elements and compounds

The effect of a dense plasma environment on the energy levels of an embedded ion is usually described in terms of the lowering of its continuum level. For strongly coupled plasmas, the phenomenon is intimately related to the equation of state; hence, an accurate treatment is crucial for most astrophysical and inertial-fusion applications, where the case of plasma mixtures is of particular interest. Here we present an experiment showing that the standard density-dependent analytical models are inadequate to describe solid-density plasmas at the temperatures studied, where the reduction of the binding energies for a given species is unaffected by the different plasma environment (ion density) in either the element or compounds of that species, and can be accurately estimated by calculations only involving the energy levels of an isolated neutral atom. The results have implications for the standard approaches to the equation of state calculations121251sciescopu

Clocking femtosecond collisional dynamics via resonant X-ray spectroscopy

Electron-ion collisional dynamics is of fundamental importance in determining plasma transport properties, non-equilibrium plasma evolution and electron damage in diffraction imaging applications using bright x-ray free-electron lasers (FELs). Here we describe the first experimental measurements of ultra-fast electron impact collisional ionization dynamics using resonant core-hole spectroscopy in a solid-density magnesium plasma, created and diagnosed with the Linac Coherent Light Source x-ray FEL. By resonantly pumping the 1s ! 2p transition in highly-charged ions within an optically-thin plasma we have measured how off-resonance charge states are populated via collisional processes on femtosecond times scales. We present a collisional cross section model that matches our results and demonstrates how the cross sections are enhanced by dense-plasma effects including continuum lowering. Non-LTE (local thermodynamic equilibrium) collisional radiative simulations show excellent agreement with the experimental results, and provide new insight on collisional ionization and three-body-recombination processes in the dense plasma regime

Stimulated resonant inelastic X-ray scattering in a solid

When materials are exposed to X-ray pulses with sufficiently high intensity, various nonlinear effects can occur. The most fundamental one consists of stimulated electronic decays after resonant absorption of X-rays. Such stimulated decays enhance the number of emitted photons and the emission direction is confined to that of the stimulating incident photons which clone themselves in the process. Here we report the observation of stimulated resonant elastic (REXS) and inelastic (RIXS) X-ray scattering near the cobalt L3 edge in solid Co/Pd multilayer samples. We observe an enhancement of order 106 of the stimulated over the conventional spontaneous RIXS signal into the small acceptance angle of the RIXS spectrometer. We also find that in solids both stimulated REXS and RIXS spectra contain contributions from inelastic electron scattering processes, even for ultrashort 5 fs pulses. Our results reveal the potential and caveats of the development of stimulated RIXS in condensed matter