Resonant soft x-ray scattering endstation for time-resolved pump-probe measurements at LCLS

Localized charge, spin and orbital degrees of freedom can compete with electronic itinerancy and such competition lies at the heart of emergent material properties. To study these electronic orderings, resonant soft X-ray scattering (RSXS) spectroscopy has been demonstrated as one of the most powerful direct probes, and its time-resolved capability can be implemented through pump-probe technique. The ultrafast/ultra-intense X-ray pulses from LCLS can be used as the probe in the time-resolved RSXS experiments, but the inherent fluctuations in intensity and timing between pulses can degrade the superior temporal resolution. To overcome such fluctuations, a compact fast CCD (cFCCD) was developed to enable shot-by-shot data acquisitions and a dedicated RSXS endstation, constructed to house this cFCCD and other single-channel photon detectors, has been extensively used at both ALS and LCLS. Time-resolved RSXS experiments on La1.75Sr0.25 NiO4 nickelate have revealed an unexpected transient behavior of charge and spin ordering (CO/SO) states. After 800nm laser excitation, the CO can be fully suppressed at higher pump fluence while SO remains detectable, creating a transient state that is not accessible by tuning thermodynamic variables. Furthermore, two distinct time scales are identified in the recovery of CO and can be attributed to the amplitude (fast) and phase (slow) dynamics of order parameter. A new version of cFCCD, with eight times the detection area and the readout electronics moved into vacuum side to minimize the pickup noise, has been developed and will be incorporated into the RSXS endstation.

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