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Snapshots of a phase transitionTime-resolved x-ray scattering can be used to investigate the dynamics of materials during the switch from one structural phase to another. So far, methods provide an ensemble average and may miss crucial aspects of the detailed mechanisms at play. Wall et al. used a total-scattering technique to probe the dynamics of the ultrafast insulator-to-metal transition of vanadium dioxide (VO2) (see the Perspective by Cavalleri). Femtosecond x-ray pulses provide access to the time- and momentum-resolved dynamics of the structural transition. Their results show that the photoinduced transition is of the order-disorder type, driven by an ultrafast change in the lattice potential that suddenly unlocks the vanadium atoms and yields large-amplitude uncorrelated motions, rather than occurring through a coherent displacive mechanism.Science, this issue p. 572; see also p. 525Many ultrafast solid phase transitions are treated as chemical reactions that transform the structures between two different unit cells along a reaction coordinate, but this neglects the role of disorder. Although ultrafast diffraction provides insights into atomic dynamics during such transformations, diffraction alone probes an averaged unit cell and is less sensitive to randomness in the transition pathway. Using total scattering of femtosecond x-ray pulses, we show that atomic disordering in photoexcited vanadium dioxide (VO2) is central to the transition mechanism and that, after photoexcitation, the system explores a large volume of phase space on a time scale comparable to that of a single phonon oscillation. These results overturn the current understanding of an archetypal ultrafast phase transition and provide new microscopic insights into rapid evolution toward equilibrium in photoexcited matter.

Excitation localization involving dynamic nanoscale distortions is a central aspect of photocatalysis 1 , quantum materials 2 and molecular optoelectronics 3 . Experimental characterization of such distortions requires techniques sensitive to the formation of point-defect-like local structural rearrangements in real time. Here, we visualize excitation-induced strain fields in a prototypical member of the lead halide perovskites 4 via femtosecond resolution diffuse X-ray scattering measurements. This enables momentum-resolved phonon spectroscopy of the locally distorted structure and reveals radially expanding nanometre-scale strain fields associated with the formation and relaxation of polarons in photoexcited perovskites. Quantitative estimates of the magnitude and shape of this polaronic distortion are obtained, providing direct insights into the dynamic structural distortions that occur in these materials 5 – 9 . Optical pump–probe reflection spectroscopy corroborates these results and shows how these large polaronic distortions transiently modify the carrier effective mass, providing a unified picture of the coupled structural and electronic dynamics that underlie the optoelectronic functionality of the hybrid perovskites. Diffuse X-ray scattering with femtosecond resolution shows the formation and relaxation of polaronic distortions in halide perovskites. These structural changes are also quantified and correlated to transient changes in carrier effective mass.

In phase-change memory devices, a material is cycled between glassy and crystalline states. The highly temperature-dependent kinetics of its crystallization process enables application in memory technology, but the transition has not been resolved on an atomic scale. Using femtosecond x-ray diffraction and ab initio computer simulations, we determined the time-dependent pair-correlation function of phase-change materials throughout the melt-quenching and crystallization process.We found a liquid–liquid phase transition in the phase-change materials Ag₄In₃Sb67Te26 and Ge15Sb85 at 660 and 610 kelvin, respectively. The transition is predominantly caused by the onset of Peierls distortions, the amplitude of which correlates with an increase of the apparent activation energy of diffusivity. This reveals a relationship between atomic structure and kinetics, enabling a systematic optimization of the memory-switching kinetics.

There is growing interest in using ultrafast light pulses to drive functional materials into nonequilibrium states with novel properties. The conventional wisdom is that above-gap photoexcitation behaves similarly to raising the electronic temperature and lacks the desired selectivity in the final state. Here, we report a novel nonthermal lattice instability induced by ultrafast above-gap excitation in SnSe, a representative of theIV−VIclass of semiconductors that provides a rich platform for tuning material functionality with ultrafast pulses due to their multiple lattice instabilities. The new lattice instability is accompanied by a drastic softening of the lowest-frequencyAgphonon. This mode has previously been identified as the soft mode in the thermally driven phase transition to aCmcmstructure. However, by a quantitative reconstruction of the atomic displacements from time-resolved x-ray diffraction for multiple Bragg peaks and excitation densities, we show that ultrafast photoexcitation with near-infrared (1.55 eV) light induces a distortion toward a different structure withImmmsymmetry. TheImmmstructure of SnSe is an orthorhombic distortion of the rocksalt structure and does not occur in equilibrium. Density functional theory calculations reveal that the photoinducedImmmlattice instability arises from electron excitation from the Se4p- and Sn5s-derived bands deep below the Fermi level that cannot be excited thermally. The results have implications for optical control of the thermoelectric, ferroelectric, and topological properties of the monochalcogenides and related materials. More generally, the results emphasize the need for ultrafast structural probes to reveal distinct atomic-scale dynamics that are otherwise too subtle or invisible in conventional spectroscopies.

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic length scales. Our results provide direct evidence that ultrafast excitation of LaTe 3 leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

We demonstrate that the absorption of femtosecond hard x-ray pulses excites quasispherical, high-amplitude, and high-wave-vector coherent acoustic phonon wave packets using an all hard-x-ray pump-probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with an ensemble of 3D strain wave packets induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the stress field and the photon energy conversion efficiency into elastic energy. The parameters are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO 3 and KTaO 3 single crystals, respectively. The results provide crucial information on the mechanism of x-ray energy deposition into matter and shed light on the shortest collective length scales accessible to coherent acoustic phonon generation using x-ray excitation.

Over the past few years, x-ray free-electron lasers (FELs) have demonstrated the possibility for probing materials with femtosecond time resolution and Angstrom spatial sensitivity. Here, we review a novel development of Fourier transform inelastic x-ray scattering (FT-IXS), which exploits the ultrafast pulses from an FEL to capture frozen snapshots of the lattice vibrations at multiple length scales simultaneously, as they oscillate when excited by a short laser pulse. This article includes an overview of the principle behind this method and a review of recent work that uses this technique to access microscopic, wave vector-dependent information on how electrons couple to the lattice and to capture phonon–phonon scattering events in real time.

The charge density wave in (TaSe 4 ) 2 I has drawn much attention recently as a controversial candidate for an axion insulator where the CDW breaks the chiral symmetry of the Weyl semimetal. Here we use ultrafast x-ray scattering to study the collective modes of this CDW. By measuring several diffraction peaks we find that the order parameter involves coupled optical and acoustic modes. For strong near-infrared excitation, the dynamics of the x-ray diffraction show evidence of photoinduced inversion of both components of the CDW order parameter, and associated domain walls. These results demonstrate the potential of ultrafast methods to induce topological defects through highly nonequilibrium dynamics. In (TaSe 4 ) 2 I these defects should lead to exotic electronic states due to the nontrivial topology of the band structure.

Time-resolved X-ray diffraction from Ga 091 Mn 0 09 As was recorded with a hard X-ray free-electron-laser. The influence of spin-orders on phonons was investigated; our result suggests a new method for mapping the spin-correlations in low doped magnetic systems, especially the short-range spin-correlation.

Predicting practical rates of transport in condensed phases enables the rational design of materials, devices and processes. This is especially critical to developing low-carbon energy technologies such as rechargeable batteries 1 – 3 . For ionic conduction, the collective mechanisms 4 , 5 , variation of conductivity with timescales 6 – 8 and confinement 9 , 10 , and ambiguity in the phononic origin of translation 11 , 12 , call for a direct probe of the fundamental steps of ionic diffusion: ion hops. However, such hops are rare-event large-amplitude translations, and are challenging to excite and detect. Here we use single-cycle terahertz pumps to impulsively trigger ionic hopping in battery solid electrolytes. This is visualized by an induced transient birefringence, enabling direct probing of anisotropy in ionic hopping on the picosecond timescale. The relaxation of the transient signal measures the decay of orientational memory, and the production of entropy in diffusion. We extend experimental results using in silico transient birefringence to identify vibrational attempt frequencies for ion hopping. Using nonlinear optical methods, we probe ion transport at its fastest limit, distinguish correlated conduction mechanisms from a true random walk at the atomic scale, and demonstrate the connection between activated transport and the thermodynamics of information. Single-cycle terahertz pumps are used to impulsively trigger ionic hopping in battery solid electrolytes, probing ion transport at its fastest limit and demonstrating the connection between activated transport and the thermodynamics of information.