We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromagnetic reorientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases.
The dynamics of an order parameter's amplitude and phase determines the collective behaviour of novel states emerging in complex materials. Time-and momentum-resolved pump-probe spectroscopy, by virtue of measuring material properties at atomic and electronic time scales out of equilibrium, can decouple entangled degrees of freedom by visualizing their corresponding dynamics in the time domain. Here we combine time-resolved femotosecond optical and resonant X-ray diffraction measurements on charge ordered La 1.75 sr 0.25 nio 4 to reveal unforeseen photoinduced phase fluctuations of the charge order parameter. such fluctuations preserve long-range order without creating topological defects, distinct from thermal phase fluctuations near the critical temperature in equilibrium. Importantly, relaxation of the phase fluctuations is found to be an order of magnitude slower than that of the order parameter's amplitude fluctuations, and thus limits charge order recovery. This new aspect of phase fluctuations provides a more holistic view of the phase's importance in ordering phenomena of quantum matter.
The designs of a compact, fast CCD (cFCCD) camera, together with a resonant soft x-ray scattering endstation, are presented. The cFCCD camera consists of a highly parallel, custom, thick, high-resistivity CCD, readout by a custom 16-channel application specific integrated circuit to reach the maximum readout rate of 200 frames per second. The camera is mounted on a virtual-axis flip stage inside the RSXS chamber. When this flip stage is coupled to a differentially pumped rotary seal, the detector assembly can rotate about 100°/360° in the vertical/horizontal scattering planes. With a six-degrees-of-freedom cryogenic sample goniometer, this endstation has the capability to detect the superlattice reflections from the electronic orderings showing up in the lower hemisphere. The complete system has been tested at the Advanced Light Source, Lawrence Berkeley National Laboratory, and has been used in multiple experiments at the Linac Coherent Light Source, SLAC National Accelerator Laboratory.
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