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Ultrafast photoinduced phase transitions at room temperature, driven by a single laser shot and persisting long after stimuli, represent emerging routes for ultrafast control over materials’ properties. Time-resolved studies provide fundamental mechanistic insight into far-from-equilibrium electronic and structural dynamics. Here we study the photoinduced phase transformation of the Rb 0.94 Mn 0.94 Co 0.06 [Fe(CN) 6 ] 0.98 material, designed to exhibit a 75 K wide thermal hysteresis around room temperature between Mn III Fe II tetragonal and Mn II Fe III cubic phases. We developed a specific powder sample streaming technique to monitor by ultrafast X-ray diffraction the structural and symmetry changes. We show that the photoinduced polarons expand the lattice, while the tetragonal-to-cubic photoinduced phase transition occurs within 100 ps above threshold fluence. These results are rationalized within the framework of the Landau theory of phase transition as an elastically-driven and cooperative process. We foresee broad applications of the streaming powder technique to study non-reversible and ultrafast dynamics. Photoinduced phase transitions occur in a variety of materials and allow for the optical control of the materials properties. Here, Herve et al present a streaming powder X-ray diffraction method allowing them to study the ultrafast photoinduced phase transition of Rb 0.94 Mn 0.94 Co 0.06 [Fe(CN) 6 ] 0.9 within thermal hysteresis.

Knowledge of the temperature dependence of the isobaric specific heat (Cp) upon deep supercooling can give insights regarding the anomalous properties of water. If a maximum in Cp exists at a specific temperature, as in the isothermal compressibility, it would further validate the liquid–liquid critical point model that can explain the anomalous increase in thermodynamic response functions. The challenge is that the relevant temperature range falls in the region where ice crystallization becomes rapid, which has previously excluded experiments. Here, we have utilized a methodology of ultrafast calorimetry by determining the temperature jump from femtosecond X-ray pulses after heating with an infrared laser pulse and with a sufficiently long time delay between the pulses to allow measurements at constant pressure. Evaporative cooling of ∼15-μm diameter droplets in vacuum enabled us to reach a temperature down to ∼228 K with a small fraction of the droplets remaining unfrozen. We observed a sharp increase in Cp, from 88 J/mol/K at 244 K to about 218 J/mol/K at 229 K where a maximum is seen. The Cp maximum is at a similar temperature as the maxima of the isothermal compressibility and correlation length. From the Cp measurement, we estimated the excess entropy and self-diffusion coefficient of water and these properties decrease rapidly below 235 K.

Recently developed ceramic material Ti 3 O 5 exhibits fascinating application properties, from ultrafast switching between metallic and insulating phases to light-to-heat conversion and storage. While the states conferring such properties are not spatially homogeneous, the origin of phase separation and the link between the phase coexistence and dynamics, key for stability of such states, is still little known. In this work, we use time-resolved X-ray diffraction and numerical simulations to establish rules by which the dynamics of heat-driven transition in laser excited Ti 3 O 5 crystallites occur in space and time. The studies are conducted on submicron Ti 3 O 5 crystallites and span a broad timescale allowing separation of phase change regimes. Our results reveal the influence of nanoscopic morphology on the mechanism of macroscopic transformation triggered by laser excitation. Ti3O5 can switch between metallic and insulating phases but its origin and the link between the phase coexistence and dynamics remain unknown. Here, time-resolved X-ray diffraction and numerical simulations were used to observe how heat-driven transition in laser excited Ti3O5 crystallites occur in space and time.

The layered transition-metal dichalcogenide WTe2 is characterized by distinctive transport and topological properties. These properties are largely determined by electronic states close to the Fermi level, specifically to electron and hole pockets in the Fermi sea. In principle, these states can be manipulated by changes to the crystal structure. The precise impact of particular structural changes on the electronic properties is a strong function of the specific nature of the atomic displacements. Here, we report on time-resolved X-ray diffraction and infrared reflectivity measurements of the coherent structural dynamics in WTe2 induced by femtosecond laser pulses excitation (central wavelength 800 nm), with emphasis on a quantitative description of both in-plane and out-of-plane vibrational modes. We estimate the magnitude of these motions, and calculate via density functional theory their effect on the electronic structure. Based on these results, we predict that phonons periodically modulate the effective mass of carriers in the electron and hole pockets up to 20%. This work opens up new opportunities for modulating the peculiar transport properties of WTe2 on short time scales.

Photoinduced charge-transfer is an important process in nature and technology and is responsible for the emergence of exotic functionalities, such as magnetic order for cyanide-bridged bimetallic coordination networks. Despite its broad interest and intensive developments in chemistry and material sciences, the atomic-scale description of the initial photoinduced process, which couples intermetallic charge-transfer and spin transition, has been debated for decades; it has been beyond reach due to its extreme speed. Here we study this process in a prototype cyanide-bridged CoFe system by femtosecond X-ray and optical absorption spectroscopies, enabling the disentanglement of ultrafast electronic and structural dynamics. Our results demonstrate that it is the spin transition that occurs first on the Co site within ~50 fs, and it is this that drives the subsequent Fe-to-Co charge-transfer within ~200 fs. This study represents a step towards understanding and controlling charge-transfer-based functions using light.Cyanide-bridged CoFe coordination networks exhibit photomagnetism because of coupled charge-transfer and spin transition. Now, femtosecond X-ray and optical absorption spectroscopies have enabled the electronic and structural dynamics of this light-induced process to be disentangled and show that it is the spin transition on the cobalt atom, occurring within ~50 fs, that induces the Fe-to-Co charge-transfer within ~200 fs.

We present the first lasing results of SwissFEL, a hard X-ray free-electron laser (FEL) that recently came into operation at the Paul Scherrer Institute in Switzerland. SwissFEL is a very stable, compact and cost-effective X-ray FEL facility driven by a low-energy and ultra-low-emittance electron beam travelling through short-period undulators. It delivers stable hard X-ray FEL radiation at 1-Å wavelength with pulse energies of more than 500 μJ, pulse durations of ~30 fs (root mean square) and spectral bandwidth below the per-mil level. Using special configurations, we have produced pulses shorter than 1 fs and, in a different set-up, broadband radiation with an unprecedented bandwidth of ~2%. The extremely small emittance demonstrated at SwissFEL paves the way for even more compact and affordable hard X-ray FELs, potentially boosting the number of facilities worldwide and thereby expanding the population of the scientific community that has access to X-ray FEL radiation.The first lasing results at SwissFEL, an X-ray free-electron laser, are presented, highlighting the facility’s unique capabilities. A general comparison to other major facilities is also provided.

Optical-domain transient grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique that is used to probe vibrational, magnetic and electronic degrees of freedom in the time domain1. The newly developed coherent X-ray free-electron laser sources allow its extension to the X-ray regime. X-rays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element specificity can address core excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. Here, we demonstrate TG excitation in the hard X-ray range at 7.1 keV. In bismuth germanate (BGO), the non-resonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods.A four-wave mixing technique is developed in the hard X-ray range. A diamond phase grating in an X-ray beam path creates a periodic excitation pattern on a sample via the Talbot effect. The response of the periodic excitation is probed by an optical pulse.

Photosystem I (PS I) has a symmetric structure with two highly similar branches of pigments at the center that are involved in electron transfer, but shows very different efficiency along the two branches. We have determined the structure of cyanobacterial PS I at room temperature (RT) using femtosecond X-ray pulses from an X-ray free electron laser (XFEL) that shows a clear expansion of the entire protein complex in the direction of the membrane plane, when compared to previous cryogenic structures. This trend was observed by complementary datasets taken at multiple XFEL beamlines. In the RT structure of PS I, we also observe conformational differences between the two branches in the reaction center around the secondary electron acceptors A 1A and A 1B . The π-stacked Phe residues are rotated with a more parallel orientation in the A-branch and an almost perpendicular confirmation in the B-branch, and the symmetry breaking PsaB-Trp673 is tilted and further away from A 1A . These changes increase the asymmetry between the branches and may provide insights into the preferential directionality of electron transfer.

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods.