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At least 1,405 records · Page 78

Observation of a mixed close-packed structure in superionic water

The study of superionic (SI) water has been a highly active research area since its theoretical prediction. Despite significant experimental and computational efforts, its melting curve and the stability of different oxygen lattices remain debated, impacting our understanding of SI ice’s peculiar transport properties. Experimental results at lower pressures show disagreement, whereas data at higher pressures are scarce due to the extreme challenges of such experiments. In this work, we present ultrafast X-ray diffraction results of water compressed by multiple shocks to pressures up to ~ 180 GPa. At pressures exceeding 150 GPa and temperatures around 2500 K, our diffraction patterns challenge the pure FCC-SI phase model, providing experimental evidence of the mixed close-packed superionic phase predicted by advanced ab initio calculations. At lower pressures, we observe simultaneous signatures of BCC and FCC structures within a pressure-temperature range consistent with some static-compression experiments, helping to resolve contradictory results in literature. These insights offer new constraints on the stability domains of SI phases and reveal detailed structural features, such as stacking faults. Our results advance the structural understanding of high-pressure SI ice to a level approaching that of ice I polymorphs, with potential implications for water-rich interiors of giant planets.

Andriambariarijaona, Leon [Centre National de la R↗

Multi-messenger dynamic imaging of laser-driven shocks in water using a plasma wakefield accelerator

Understanding dense matter hydrodynamics is critical for predicting plasma behavior in environments relevant to laser-driven inertial confinement fusion. Traditional diagnostic sources face limitations in brightness, spatiotemporal resolution, and in their ability to detect relevant electromagnetic fields. In this work, we present a dual-probe, multi-messenger laser wakefield accelerator platform combining ultrafast X-rays and relativistic electron beams at 1 Hz, to interrogate a free-flowing water target in vacuum, heated by an intense 200 ps laser pulse. This scheme enables high-repetition-rate tracking the evolution of the interaction using both particle types. Betatron X-rays reveal a cylindrically symmetric shock compression morphology assisted by low-density vapor, resembling foam-layer-assisted fusion targets. The synchronized electron beam detects time-evolving electromagnetic fields, uncovering charge separation and ion species differentiation during plasma expansion – phenomena not captured by photons or hydrodynamic simulations. We show that combining both probes provides complementary insights spanning kinetic to hydrodynamic regimes, highlighting the need for hybrid physics models to accurately predict fusion-relevant plasma behavior.

imaging techniques↗

Topological magneto-optical Kerr effect without spin-orbit coupling in spin-compensated antiferromagnet

The magneto-optical Kerr effect (MOKE), the differential reflection of oppositely circularly polarized light, has traditionally been associated with relativistic spin-orbit coupling (SOC), which links a particle’s spin with its orbital motion. In ferromagnets, large MOKE signals arise from the combination of magnetization and SOC, while in certain coplanar antiferromagnets, SOC-induced Berry curvature enables MOKE despite zero net magnetization. Theoretically, large MOKE can also arise in a broader class of magnetic materials with compensated spins, without relying on SOC - for example, in systems exhibiting real-space scalar spin chirality. The experimental verification has remained elusive. Here, we demonstrate such a SOC- and magnetization-free MOKE in the noncoplanar antiferromagnet Co 1/3 TaS 2 . Using a Sagnac interferometer microscope, we image domains of scalar spin chirality and their reversal. Our findings establish experimentally a new mechanism for generating large MOKE signals and position chiral spin textures in compensated magnets as a compelling platform for ultrafast, stray-field-immune opto-spintronic applications.

Magnetic properties and materials↗

Photoinduced correlations in stochastic dynamics of a solid-state ionic conductor

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and probing complex molecular dynamics. The photoresponse following a laser pulse is generally nonidentical between exposures due to spatiotemporal fluctuations or the stochastic nature of dynamical pathways. However, most ultrafast pump-probe experiments struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing deviations from the averaged response. Leveraging the stability and high photon flux of time-resolved X-ray micro-diffraction at a synchrotron, we characterized stochastic photoinduced dynamics in a solid-state ionic conductor. By analyzing temporal evolutions of the lattice parameter of a single grain, we found that shot-to-shot fluctuations are not independent. Instead, correlations exist between nonequilibrium lattice trajectories following adjacent shots, with a characteristic correlation length of approximately 1500 shots, corresponding to an energy barrier of 0.4 ± 0.1 eV, close to the activation energy of lithium-ion diffusion.

36 MATERIALS SCIENCE↗

Electron-ion equilibration in superheated gold

Electron-ion equilibration dynamics in samples driven into superheated states with multi-eV electron temperatures represent a fundamental process in nonequilibrium physics. A clear picture of the evolving ion temperature is essential for understanding the strength of the electron-ion coupling. However, direct, model-independent measurements of the ion temperature in laser-irradiated samples have remained experimentally elusive. Using inelastic X-ray scattering with meV-resolution in gold samples, the ion response to ultrafast heating by the hot electrons can be resolved, quantifying the electron-ion equilibration dynamics. We report measurements revealing a strongly enhanced energy transfer rate compared to that in weakly excited gold. Moreover, we obtain a quasi-constant electron-ion coupling at the highly elevated electron temperatures. These results place new constraints on electron-ion energy transfer in warm dense matter and establish a path toward quantitative benchmarking of models for nonequilibrium dynamics.

Griffin, Travis D. [Univ. of Nevada, Reno, NV (Uni↗

Signatures of nonthermal carriers in nonlinear photoluminescence

Ultrafast light emission from plasmonic nanostructures provides a sensitive probe of the energetic electrons generated by intense optical excitation. The way this emission scales with excitation intensity has long been read through the lens of heated electron populations at an elevated temperature, yet this picture cannot reconcile the variety of behaviors seen across different materials and experiments. We argue that transient nonthermal electrons play a far larger role than has been appreciated. We present a unified description that reproduces emission behavior across diverse systems and outline experiments needed to resolve their signatures.

nanoscale materials↗

The critical role of hot carrier cooling in optically excited structural transitions

The hot carrier cooling occurs in most photoexcitation-induced phase transitions (PIPTs), but its role has often been neglected in many theoretical simulations as well as in proposed mechanisms. Here, by including the previously ignored hot carrier cooling in real-time time-dependent density functional theory (rt-TDDFT) simulations, we investigated the role of hot carrier cooling in PIPTs. Taking IrTe2 as an example, we reveal that the cooling of hot electrons from the higher energy levels of spatially extended states to the lower energy levels of the localized Ir–Ir dimer antibonding states strengthens remarkably the atomic driving forces and enhances atomic kinetic energy. These two factors combine to dissolute the Ir–Ir dimers on a timescale near the limit of atomic motions, thus initiating a deterministic kinetic phase transition. We further demonstrate that the subsequent cooling induces nonradiative recombination of photoexcited electrons and holes, leading to the ultrafast recovery of the Ir–Ir dimers observed experimentally. These findings provide a complete picture of the atomic dynamics in optically excited structural phase transitions.

36 MATERIALS SCIENCE↗

Circumventing the phonon bottleneck by multiphonon-mediated hot exciton cooling at the nanoscale

Abstract Nonradiative processes govern efficiencies of semiconductor nanocrystal (NC)-based devices. A central process is hot exciton cooling, or the nonradiative relaxation of a highly excited electron/hole pair to form a band-edge exciton. Due to quantum confinement effects, the timescale and mechanism of cooling are not well understood. A mismatch between electronic energy gaps and phonon frequencies has led to the hypothesis of a phonon bottleneck and extremely slow cooling, while enhanced electron-hole interactions have suggested ultrafast cooling. Experimental measurements of the cooling timescale range six orders of magnitude. Here, we develop an atomistic approach to describe phonon-mediated exciton dynamics and simulate cooling in NCs of experimentally relevant sizes. We find that cooling occurs on ~30 fs timescales in CdSe NCs, in agreement with the most recent measurements, and that the phonon bottleneck is circumvented through a cascade of multiphonon-mediated relaxation events. Furthermore, we identify NC handles for tuning the cooling timescale.

36 MATERIALS SCIENCE↗

Advancing simulations of coupled electron and phonon nonequilibrium dynamics using adaptive and multirate time integration

Electronic structure calculations in the time domain provide a deeper understanding of nonequilibrium dynamics in materials. The real-time Boltzmann equation (rt-BTE), used in conjunction with accurate interactions computed from first principles, has enabled reliable predictions of coupled electron and lattice dynamics. However, the timescales and system sizes accessible with this approach are still limited, with two main challenges being the different timescales of electron and phonon interactions and the cost of computing collision integrals. As a result, only a few examples of these calculations exist, mainly for two-dimensional (2D) materials. Here we leverage adaptive and multirate time integration methods to achieve a major step forward in solving the coupled rt-BTEs for electrons and phonons. Relative to conventional (non-adaptive) time-stepping, our approach achieves a 10x speedup for a target accuracy, or greater accuracy by 3–6 orders of magnitude for the same computational cost, enabling efficient calculations in both 2D and bulk materials. This efficiency is showcased by computing the coupled electron and lattice dynamics in graphene up to ~100 ps, as well as modeling ultrafast lattice dynamics and thermal diffuse scattering maps in bulk materials (silicon and gallium arsenide). In addition to improved efficiency, our adaptive method can resolve the characteristic rates of different physical processes, thus naturally bridging different timescales. This enables simulations of longer timescales and provides a framework for modeling multiscale dynamics of coupled degrees of freedom in matter. Our work opens new opportunities for quantitative studies of nonequilibrium physics in materials, including driven lattice dynamics with phonons coupled to electrons, spin, and other degrees of freedom.

Yao, Jia [California Institute of Technology (CalT↗

In situ electron microscopy: atomic-scale dynamics of metal oxidation and corrosion

Corrosion degrades metals through complex microscopic processes that traditional methods often fail to capture. In-situ transmission electron microscopy (TEM) bridges this gap by providing real-time atomic-scale imaging of oxidation and corrosion dynamics. Gas-phase TEM uncovers critical oxidation mechanisms like oxide nucleation and alloying effects, while liquid-phase TEM tracks corrosion initiation. Coupled with emerging techniques like ultrafast direct electron detection cameras, these advancements promise unprecedented resolution in understanding material degradation.

36 MATERIALS SCIENCE↗

Probing the interplay between lattice dynamics and short-range magnetic correlations in CuGeO 3 with femtosecond RIXS

Investigations of magnetically ordered phases on the femtosecond timescale have provided significant insights into the influence of charge and lattice degrees of freedom on the magnetic sub-system. However, short-range magnetic correlations occurring in the absence of long-range order, for example in spin-frustrated systems, are inaccessible to many ultrafast techniques. Here, we show how time-resolved resonant inelastic X-ray scattering (trRIXS) is capable of probing such short-ranged magnetic dynamics in a charge-transfer insulator through the detection of a Zhang–Rice singlet exciton. Utilizing trRIXS measurements at the O K-edge, and in combination with model calculations, we probe the short-range spin correlations in the frustrated spin chain material CuGeO 3 following photo-excitation, revealing a strong coupling between the local lattice and spin sub-systems.

36 MATERIALS SCIENCE↗

Photoinduced evolution of lattice orthorhombicity and conceivably enhanced ferromagnetism in LaMnO 3 membranes

Ultrashort laser pulses have been utilized to dynamically drive phase transitions in correlated quantum materials. Of particular interest is whether phases not achievable in thermal equilibrium can be induced in complex oxides with intricately coupled lattice, electron and spin degrees of freedom. Here, we tracked atomic motions in LaMnO 3 following photoexcitation with MeV ultrafast electron diffraction (MeV-UED) technique. We found that the light excited state exhibits numerous signatures different from thermal equilibrium ones, including nearly conserved Bragg intensities, strongly suppressed La cation and oxygen anion displacements, and the long-range lattice orthorhombicity evolution. Furthermore, using first-principles calculations, we predict that the ferromagnetic ordering and conductivity are both enhanced upon laser excitation due to the reduction of the lattice orthorhombicity. This work benefits from recent advance in fabrication of membrane films with high epitaxial quality and in MeV-UED with large momentum space access and high temporal resolution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Vibronic coupling-driven symmetry breaking and solvation in the photoexcited dynamics of quadrupolar dyes

Quadrupolar dyes, such as acceptor–donor–acceptor molecules, are highly relevant for applications in nonlinear optics and photovoltaics. They are also versatile models for exploring photoinduced charge-transfer dynamics. The interplay between electronic and vibronic couplings in these molecules may break excited-state symmetry, resulting in intramolecular charge separation and pronounced solvatochromism. Experimentally, distinguishing the roles of intramolecular vibronic coupling and solvent reorganization for the initial charge-transfer dynamics has been challenging so far. Here we investigate a prototypical quadrupolar dye in polar and non-polar solvents using ultrafast pump–probe and two-dimensional electronic spectroscopy. Our results reveal that vibronic couplings initiate excited-state symmetry breaking during the first ~50 fs of the photoinduced charge transfer, whereas solvent-induced charge localization sets in at later times. Quantum dynamics and electronic structure simulations support our experimental findings. Our results reveal the details of solvation dynamics in photoexcited molecules and suggest strategies for their manipulation through vibronic couplings.

36 MATERIALS SCIENCE↗

Chirality-induced spin selectivity as a mechanism to control product selectivity during electrochemical CO 2 reduction

Electrocatalytic CO 2 reduction often suffers from competition with the hydrogen evolution reaction (HER), which lowers efficiency and limits product selectivity. Recent studies suggest that electron spin, when controlled at an electrode surface, can influence reaction pathways, but direct evidence linking spin effects to suppressed HER has been limited. Here, in this work, we show that helical chiral copper (Cu) electrodes reduce competing HER during CO 2 reduction, consistent with spin polarization induced via the chiral-induced spin selectivity effect. The helically structured Cu electrodes are fabricated by electrodeposition with a chiral templating reagent. Time-resolved Kerr ellipticity measurements, which track spin-polarized carriers generated by an ultrafast Seebeck current, confirm spin accumulation at the chiral Cu surface. This spin polarization disfavours H—H bond formation, thereby suppressing HER and enabling formate production alongside CO. These findings demonstrate that chirality-based spin control offers a strategy for steering selectivity in CO 2 reduction and other reactions where HER is an undesired competitor.

14 SOLAR ENERGY↗

Evidence for d -wave superconductivity of infinite-layer nickelates from low-energy electrodynamics

The discovery of superconductivity in infinite-layer nickelates established another category of unconventional superconductors that shares structural and electronic similarities with cuprates. However, key issues of the superconducting pairing symmetry, gap amplitude and superconducting fluctuations are yet to be addressed. Here we utilize static and ultrafast terahertz spectroscopy to address these. We demonstrate that the equilibrium terahertz conductivity and non-equilibrium terahertz responses of an optimally Sr-doped nickelate film (superconducting transition temperature of T c = 17 K) are in line with the electrodynamics of d-wave superconductivity in the dirty limit. The gap-to-T c ratio (2Δ/k B T c ) is found to be 3.4, indicating that the superconductivity falls in the weak coupling regime. In addition, we observed substantial superconducting fluctuations near T c that do not extend into the deep normal state as the optimally hole-doped cuprates do. In conclusion, our results support a d-wave system that closely resembles the electron-doped cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Exciton polaron formation and hot-carrier relaxation in rigid Dion–Jacobson-type two-dimensional perovskites

The efficiency of two-dimensional Dion–Jacobson-type materials relies on the complex interplay between electronic and lattice dynamics; however, questions remain about the functional role of exciton–phonon interactions. Here we establish the robust polaronic nature of the excitons in these materials at room temperature by combining ultrafast spectroscopy and electronic structure calculations. We show that polaronic distortion is associated with low-frequency (30–60 cm –1 ) lead iodide octahedral lattice motions. More importantly, we discover how targeted ligand modification of this two-dimensional perovskite structure manipulates exciton–phonon coupling, exciton polaron population and carrier cooling. At high excitation density, stronger exciton–phonon coupling increases the hot-carrier lifetime, forming a hot-phonon bottleneck. Furthermore, our study provides detailed insight into the exciton–phonon coupling and its role in carrier cooling in two-dimensional perovskites relevant for developing emerging hybrid semiconductor materials with tailored properties.

36 MATERIALS SCIENCE↗

Correlated spin-wave generation and domain-wall oscillation in a topologically textured magnetic film

Spin waves, or magnons, are essential for next-generation energy-efficient spintronics and magnonics. Yet, visualizing spin-wave dynamics at nanoscale and microwave frequencies remains a formidable challenge due to the lack of spin-sensitive, time-resolved microscopy. Here, in this study, we report a breakthrough in imaging dipole-exchange spin waves in a ferromagnetic film owing to the development of laser-free ultrafast Lorentz electron microscopy, which is equipped with a microwave-mediated electron pulser for high spatiotemporal resolution. Using topological spin textures, we captured the emission, propagation, reflection and interference of spin waves from spin anti-vortices under radio-frequency excitations. Remarkably, we show that spin-wave generation is closely tied to the oscillatory motion of specific magnetic domain walls, providing the missing link between wave emission and wall dynamics near magnetic singularities. This work opens new possibilities in magnonics, offering a nanoscopic view of spin dynamics via transmission electron microscopy and enabling controlled excitation via radio-frequency fields for exploring non-equilibrium states in magnetic and multiferroic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Protonic nickelate device networks for spatiotemporal neuromorphic computing

Computation in biological neural circuits arises from the interplay of nonlinear temporal responses and spatially distributed dynamic network interactions. Replicating this richness in hardware has remained challenging, as most neuromorphic devices emulate only isolated neuron- or synapse-like functions. Here we introduce an integrated neuromorphic computing platform in which both nonlinear spatiotemporal processing and programmable memory are realized within a single perovskite nickelate material system. By engineering symmetric and asymmetric hydrogenated NdNiO 3 junction devices on the same wafer, we combine ultrafast, proton-mediated transient dynamics with stable multilevel resistance states. Networks of symmetric NdNiO 3 junctions exhibit emergent spatial interactions mediated by proton redistribution, while each node simultaneously provides short-term temporal memory, enabling nanosecond-scale operation with an energy cost of ~0.2 nJ per input. When interfaced with asymmetric output units serving as reconfigurable long-term weights, these networks allow both feature transformation and linear classification in the same material system. Leveraging these emergent interactions, the platform enables real-time pattern recognition and achieves high accuracy in spoken digit classification and early seizure detection, outperforming temporal-only or uncoupled architectures. These results position protonic nickelates as a compact, energy-efficient, CMOS-compatible platform that integrates processing and memory for scalable intelligent hardware.

Electrical and electronic engineering↗