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We have developed a timing control system to stabilize the long‐term timing drift between X‐ray free‐electron laser (XFEL) and optical laser pulses using an out‐of‐loop balanced optical‐microwave phase detector and an arrival‐timing monitor for pump–probe experiments at the SPring‐8 Ångstrom Compact free‐electron LAser (SACLA). The timing jitter and drift between the XFEL and the optical laser pulses have been reduced to less than 50 fs (RMS) over ∼49 h. The performance of the timing stabilization system was investigated by measuring the correlation of the long‐term simultaneous timing monitoring on two branches of BL3 over 8 h. A linear correlation was observed with an RMS error of 8.6 fs. A timing control system to stabilize the long‐term timing drift between X‐ray free‐electron laser (XFEL) and optical laser pulses has been developed by utilizing an out‐of‐loop balanced optical‐microwave phase detector and an arrival‐timing monitor. The timing jitter and drift between the XFEL and the optical laser pulses have been reduced to less than 50 fs (RMS) over ∼49 h.

Disentangling the strong interplay between electronic and nuclear degrees of freedom is essential to achieve a full understanding of excited state processes during ultrafast nonadiabatic chemical reactions. However, the complexity of multi-dimensional potential energy surfaces means that this remains challenging. The energy flow during vibrational and electronic relaxation processes can be explored with structural sensitivity by probing a nuclear wavepacket using femtosecond time-resolved X-ray Absorption Near Edge Structure (TR-XANES). However, it remains unknown to what level of detail vibrational motions are observable in this X-ray technique. Herein we track the wavepacket dynamics of a prototypical [Cu(2,9-dimethyl-1,10-phenanthroline) 2 ] + complex using TR-XANES. We demonstrate that sensitivity to individual wavepacket components can be modulated by the probe energy and that the bond length change associated with molecular breathing mode can be tracked with a sub-Angstrom resolution beyond optical-domain observables. Importantly, our results reveal how state-of-the-art TR-XANES provides deeper insights of ultrafast nonadiabatic chemical reactions. Nonadiabatic excited state processes involve mixing of electronic and nuclear wavefunctions, which are difficult to disentangle. Here the authors explore by time-resolved X-ray absorption near edge structure the wavepacket dynamics of a copper(I)-phenanthroline complex, resolving different vibrational modes.

Understanding the ultrashort time scale structural dynamics of the FeRh metamagnetic phase transition is a key element in developing a complete explanation of the mechanism driving the evolution from an antiferromagnetic to ferromagnetic state. Using an X-ray free electron laser we determine, with sub-ps time resolution, the time evolution of the (–101) lattice diffraction peak following excitation using a 35 fs laser pulse. The dynamics at higher laser fluence indicates the existence of a transient lattice state distinct from the high temperature ferromagnetic phase. By extracting the lattice temperature and comparing it with values obtained in a quasi-static diffraction measurement, we estimate the electron–phonon coupling in FeRh thin films as a function of laser excitation fluence. A model is presented which demonstrates that the transient state is paramagnetic and can be reached by a subset of the phonon bands. A complete description of the FeRh structural dynamics requires consideration of coupling strength variation across the phonon frequencies.

Meteorites from interplanetary space often include high-pressure polymorphs of their constituent minerals, which provide records of past hypervelocity collisions. These collisions were expected to occur between kilometre-sized asteroids, generating transient high-pressure states lasting for several seconds to facilitate mineral transformations across the relevant phase boundaries. However, their mechanisms in such a short timescale were never experimentally evaluated and remained speculative. Here, we show a nanosecond transformation mechanism yielding ringwoodite, which is the most typical high-pressure mineral in meteorites. An olivine crystal was shock-compressed by a focused high-power laser pulse, and the transformation was time-resolved by femtosecond diffractometry using an X-ray free electron laser. Our results show the formation of ringwoodite through a faster, diffusionless process, suggesting that ringwoodite can form from collisions between much smaller bodies, such as metre to submetre-sized asteroids, at common relative velocities. Even nominally unshocked meteorites could therefore contain signatures of high-pressure states from past collisions. Meteorites from space often include denser polymorphs of their minerals, providing records of past hypervelocity collisions. An olivine mineral crystal was shock-compressed by a high-power laser, and its transformation into denser ringwoodite was time-resolved using an X-ray free electron laser.

In this study, we use laser-driven shock compression coupled with in situ X-ray diffraction to interrogate the phase transition dynamics of shock-compressed zircon (ZrSiO 4 ) for the first time. A phase transition from zircon to the high-pressure reidite phase was observed during the nanosecond timescale of a laser-driven shock. At high laser power, diffraction peaks of zircon and reidite appeared superimposed on two broad features. This diffuse background was ascribed to liquid scattering from a partial melt. At the highest laser power, the diffuse scattering dominated, with minimal evidence for crystal diffraction. On release, the melt recrystallized into a combination of zircon and reidite. Decomposition of zircon to SiO 2 and ZrO 2 was not observed. This study revealed that on laser-shock timescales, the zircon–reidite phase transition readily occurs. However, the decomposition of zircon into ZrO 2 and SiO 2 is kinetically inhibited.

We report a method for achieving advanced photon diagnostics of x-ray free-electron lasers (XFELs) under a quasi-noninvasive condition by using a beam-splitting scheme. Here, we used a transmission grating to generate multiple branches of x-ray beams. One of the two primary diffracted branches (+1st-order) is utilized for spectral measurement in a dispersive scheme, while the other (−1st-order) is dedicated for arrival timing diagnostics between the XFEL and the optical laser pulses. The transmitted x-ray beam (0th-order) is guided to an experimental station. To confirm the validity of this timing-monitoring scheme, we measured the correlation between the arrival timings of the −1st and 0th branches. The observed error was as small as 7.0 fs in root-mean-square. Our result showed the applicability of the beam branching scheme to advanced photon diagnostics, which will further enhance experimental capabilities of XFEL.

Unraveling the origin of ultrafast demagnetization in multisublattice ferromagnetic materials requires femtosecond x-ray techniques to trace the magnetic moment dynamics on individual elements, but this could not yet be achieved in the hard x-ray regime. We demonstrate here the first ultrafast demagnetization dynamics in the ferromagnetic heavy 5d-transition metal Pt using circularly-polarized hard x-rays at an x-ray free electron laser (XFEL). The decay time of laser-induced demagnetization of L10-FePt is determined to be τ Pt = 0.61 0.04 ps using time-resolved x-ray magnetic circular dichroism at the Pt L3 edge, whereas magneto-optical Kerr measurements indicate the decay time for the total magnetization as τ total < 0.1 ps . A transient magnetic state with a photo-modulated ratio of the 3d and 5d magnetic moments is demonstrated for pump-probe delays larger than 1 ps. We explain this distinct photo-modulated transient magnetic state by the induced-moment behavior of the Pt atom and the x-ray probing depth. Our findings pave the way for the future use of XFELs to disentangle atomic spin dynamics contributions.

Crystallization is a fundamental natural phenomenon and the ubiquitous physical process in materials science for the design of new materials. So far, experimental observations of the structural dynamics in crystallization have been mostly restricted to slow dynamics. We present here an exclusive way to explore the dynamics of crystallization in highly controlled conditions (i.e., in the absence of impurities acting as seeds of the crystallites) as it occurs in vacuum. We have measured the early formation stage of solid Xe nanoparticles nucleated in an expanding supercooled Xe jet by means of an X-ray diffraction experiment with 10-fs X-ray free-electron laser (XFEL) pulses. We found that the structure of Xe nanoparticles is not pure face-centered cubic (fcc), the expected stable phase, but a mixture of fcc and randomly stacked hexagonal close-packed (rhcp) structures. Furthermore, we identified the instantaneous coexistence of the comparably sized fcc and rhcp domains in single Xe nanoparticles. The observations are explained by the scenario of structural aging, in which the nanoparticles initially crystallize in the highly stacking-disordered rhcp phase and the structure later forms the stable fcc phase. The results are reminiscent of analogous observations in hard-sphere systems, indicating the universal role of the stacking-disordered phase in nucleation.

The charge-carrier dynamics of anatase TiO2 nanoparticles in an aqueous solution were studied by femtosecond time-resolved X-ray absorption spectroscopy using an X-ray free electron laser in combination with a synchronized ultraviolet femtosecond laser (268 nm). Using an arrival time monitor for the X-ray pulses, we obtained a temporal resolution of 170 fs. The transient X-ray absorption spectra revealed an ultrafast Ti K-edge shift and a subsequent growth of a pre-edge structure. The edge shift occurred in ca. 100 fs and is ascribed to reduction of Ti by localization of generated conduction band electrons into shallow traps of self-trapped polarons or deep traps at penta-coordinate Ti sites. Growth of the pre-edge feature and reduction of the above-edge peak intensity occur with similar time constants of 300–400 fs, which we assign to the structural distortion dynamics near the surface.

Over the past century, understanding the nature of shock compression of condensed matter has been a major topic. About 20 years ago, a femtosecond laser emerged as a new shock-driver. Unlike conventional shock waves, a femtosecond laser-driven shock wave creates unique microstructures in materials. Therefore, the properties of this shock wave may be different from those of conventional shock waves. However, the lattice behaviour under femtosecond laser-driven shock compression has never been elucidated. Here we report the ultrafast lattice behaviour in iron shocked by direct irradiation of a femtosecond laser pulse, diagnosed using X-ray free electron laser diffraction. We found that the initial compression state caused by the femtosecond laser-driven shock wave is the same as that caused by conventional shock waves. We also found, for the first time experimentally, the temporal deviation of peaks of stress and strain waves predicted theoretically. Furthermore, the existence of a plastic wave peak between the stress and strain wave peaks is a new finding that has not been predicted even theoretically. Our findings will open up new avenues for designing novel materials that combine strength and toughness in a trade-off relationship.