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At least 991 records · Page 55

Photoinduced Dirac semimetal in ZrTe5

Abstract Novel phases of matter with unique properties that emerge from quantum and topological protection present an important thrust of modern research. Of particular interest is to engineer these phases on demand using ultrafast external stimuli, such as photoexcitation, which offers prospects of their integration into future devices compatible with optical communication and information technology. Here, we use MeV Ultrafast Electron Diffraction (UED) to show how a transient three-dimensional (3D) Dirac semimetal state can be induced by a femtosecond laser pulse in a topological insulator ZrTe 5 . We observe marked changes in Bragg diffraction, which are characteristic of bond distortions in the photoinduced state. Using the atomic positions refined from the UED, we perform density functional theory (DFT) analysis of the electronic band structure. Our results reveal that the equilibrium state of ZrTe 5 is a topological insulator with a small band gap of ~ 25 meV, consistent with angle-resolved photoemission (ARPES) experiments. However, the gap is closed in the presence of strong spin-orbit coupling (SOC) in the photoinduced transient state, where massless Dirac fermions emerge in the chiral band structure. The time scale of the relaxation dynamics to the transient Dirac semimetal state is remarkably long, τ ~ 160 ps, which is two orders of magnitude longer than the conventional phonon-driven structural relaxation. The long relaxation is consistent with the vanishing density of states in Dirac spectrum and slow spin-repolarization of the SOC-controlled band structure accompanying the emergence of Dirac fermions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photoinduced anisotropic lattice dynamic response and domain formation in thermoelectric SnSe

Identifying and understanding the mechanisms behind strong phonon–phonon scattering in condensed matter systems is critical to maximizing the efficiency of thermoelectric devices. To date, the leading method to address this has been to meticulously survey the full phonon dispersion of the material in order to isolate modes with anomalously large linewidth and temperature-dependence. Here we combine quantitative MeV ultrafast electron diffraction (UED) analysis with Monte Carlo based dynamic diffraction simulation and first-principles calculations to directly unveil the soft, anharmonic lattice distortions of model thermoelectric material SnSe. A small single-crystal sample is photoexcited with ultrafast optical pulses and the soft, anharmonic lattice distortions are isolated using MeV-UED as those associated with long relaxation time and large displacements. We reveal that these modes have interlayer shear strain character, induced mainly by c -axis atomic displacements, resulting in domain formation in the transient state. These findings provide an innovative approach to identify mechanisms for ultralow and anisotropic thermal conductivity and a promising route to optimizing thermoelectric devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Time-domain study of coupled collective excitations in quantum materials

Quantum materials hold immense promises for future applications due to their intriguing electronic, magnetic, thermal, and mechanical properties that often arise from a complex interplay between microscopic degrees of freedom. Important insights of such interactions come from studying the collective excitations of electrons, spins, orbitals, and lattice, whose cooperative motions play a crucial role in determining the novel behavior of these systems and offer us a key tuning knob to modify material properties on-demand through external perturbations. In this regard, ultrafast light-matter interaction has shown great potential in controlling the couplings of collective excitations, and rapid progress in a plethora of time-resolved techniques down to the attosecond regime has significantly advanced our understanding of the coupling mechanisms and guided us in manipulating the dynamical properties of quantum materials. This review aims to highlight recent experiments on visualizing collective excitations in the time domain, focusing on the coupling mechanisms between different collective modes such as phonon-phonon, phonon-magnon, phonon-exciton, magnon-magnon, magnon-exciton, and various polaritons. We introduce how these collective modes are excited by an ultrashort laser pulse and probed by different ultrafast techniques, and we explain how the coupling between collective excitations governs the ensuing nonequilibrium dynamics. We also provide some perspectives on future studies that can lead to discoveries of the emergent properties of quantum materials both in and out of equilibrium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Direct observation of coherent femtosecond solvent reorganization coupled to intramolecular electron transfer

It is well known that the solvent plays a critical role in ultrafast electron-transfer reactions. However, solvent reorganization occurs on multiple length scales, and selectively measuring short-range solute–solvent interactions at the atomic level with femtosecond time resolution remains a challenge. Here we report femtosecond X-ray scattering and emission measurements following photoinduced charge-transfer excitation in a mixed-valence bimetallic (Fe ii Ru iii ) complex in water, and their interpretation using non-equilibrium molecular dynamics simulations. Combined experimental and computational analysis reveals that the charge-transfer excited state has a lifetime of 62 fs and that coherent translational motions of the first solvation shell are coupled to the back electron transfer. Overall, our molecular dynamics simulations identify that the observed coherent translational motions arise from hydrogen bonding changes between the solute and nearby water molecules upon photoexcitation, and have an amplitude of tenths of ångströms, 120–200 cm -1 frequency and ~100 fs relaxation time. This study provides an atomistic view of coherent solvent reorganization mediating ultrafast intramolecular electron transfer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photocurrent-driven transient symmetry breaking in the Weyl semimetal TaAs

Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry changes a critical step in developing future technologies that rely on such control. Topological materials, like topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second harmonic generation spectroscopy as a sensitive probe of symmetry changes, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Here, our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast timescales.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

X-ray multiphoton-induced Coulomb explosion images complex single molecules

Following structural dynamics in real time is a fundamental goal towards a better understanding of chemical reactions. Recording snapshots of individual molecules with ultrashort exposure times is a key ingredient towards this goal, as atoms move on femtosecond (10 -15 s) timescales. For condensed-phase samples, ultrafast, atomically resolved structure determination has been demonstrated using X-ray and electron diffraction. Pioneering experiments have also started addressing gaseous samples. However, they face the problem of low target densities, low scattering cross sections and random spatial orientation of the molecules. Therefore, obtaining images of entire, isolated molecules capturing all constituents, including hydrogen atoms, remains challenging. Here we demonstrate that intense femtosecond pulses from an X-ray free-electron laser trigger rapid and complete Coulomb explosions of 2-iodopyridine and 2-iodopyrazine molecules. We obtain intriguingly clear momentum images depicting ten or eleven atoms, including all the hydrogens, and thus overcome a so-far impregnable barrier for complete Coulomb explosion imaging—its limitation on molecules consisting of three to five atoms. In combination with state-of-the-art multi-coincidence techniques and elaborate theoretical modelling, this allows tracing ultrafast hydrogen emission and obtaining information on the result of intramolecular electron rearrangement. Our work represents an important step towards imaging femtosecond chemistry via Coulomb explosion.

74 ATOMIC AND MOLECULAR PHYSICS↗

All-optical seeding of a light-induced phase transition with correlated disorder

Ultrafast manipulation of vibrational coherence is an emergent route to control the structure of solids. However, this strategy can only induce long-range correlations and cannot modify atomic structure locally, which is required in many technologically-relevant phase transitions. Here, we demonstrate that ultrafast lasers can generate incoherent structural fluctuations which are more efficient for material control than coherent vibrations, extending optical control to a wider range of materials. We observe that local, non-equilibrium lattice distortions generated by a weak laser pulse reduce the energy barrier to switch between insulating and metallic states in vanadium dioxide by 6%. In conclusion, seeding inhomogeneous structural-fluctuations presents an alternative, more energy efficient, route for controlling materials that may be applicable to all solids, including those used in data and energy storage devices.

36 MATERIALS SCIENCE↗

Attosecond response of molecules to impulsive ionization

When matter interacts with energetic radiation it can undergo sudden, or impulsive, ionization. This process can drive chemical change and occurs widely in space and planetary atmospheres, yet its comprehensive description challenges our current theoretical and computational capabilities as it requires advanced treatment of electron correlation and nonadiabatic dynamics beyond the Born–Oppenheimer approximation. Here, in this study, we measure the response of the para-aminophenol molecule to sudden ionization. Using attosecond X-ray absorption spectroscopy, we resolve the ultrafast dynamics of the ionized molecule with atomic precision. A subfemtosecond decay corresponds to states undergoing non-radiative decay, whereas few-femtosecond oscillatory signatures are associated with electronic wavepacket motion in stable cation states that later couple to nuclear motion. We compare our measurement with state-of-the-art computational modelling, qualitatively reproducing the observed response across multiple timescales. These results provide a benchmark for computational models of sudden ionization and ultrafast charge motion in matter.

Driver, Taran [SLAC National Accelerator Laborator↗

Subterahertz collective dynamics of polar vortices

The collective dynamics of topological structures are of interest from both fundamental and applied perspectives. For example, studies of dynamical properties of magnetic vortices and skyrmions have not only deepened our understanding of many-body physics but also offered potential applications in data processing and storage. Topological structures constructed from electrical polarization, rather than electron spin, have recently been realized in ferroelectric superlattices, and these are promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics underlying the functionality of such complex extended nanostructures. In this study, using terahertz-field excitation and femtosecond X-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders-of-magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices. A previously unseen tunable mode, hereafter referred to as a vortexon, emerges in the form of transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond timescales. Its frequency is considerably reduced (softened) at a critical strain, indicating a condensation (freezing) of structural dynamics. We use first-principles-based atomistic calculations and phase-field modelling to reveal the microscopic atomic arrangements and corroborate the frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens opportunities for electric-field-driven data processing in topological structures with ultrahigh speed and density.

36 MATERIALS SCIENCE↗

Light-driven nanoscale vectorial currents

Controlled charge flows are fundamental to many areas of science and technology, serving as carriers of energy and information, as probes of material properties and dynamics and as a means of revealing or even inducing broken symmetries. Emerging methods for light-based current control offer particularly promising routes beyond the speed and adaptability limitations of conventional voltage-driven systems. However, optical generation and manipulation of currents at nanometre spatial scales remains a basic challenge and a crucial step towards scalable optoelectronic systems for microelectronics and information science. Here we introduce vectorial optoelectronic metasurfaces in which ultrafast light pulses induce local directional charge flows around symmetry-broken plasmonic nanostructures, with tunable responses and arbitrary patterning down to subdiffractive nanometre scales. Local symmetries and vectorial currents are revealed by polarization-dependent and wavelength-sensitive electrical readout and terahertz (THz) emission, whereas spatially tailored global currents are demonstrated in the direct generation of elusive broadband THz vector beams 17 . We show that, in graphene, a detailed interplay between electrodynamic, thermodynamic and hydrodynamic degrees of freedom gives rise to rapidly evolving nanoscale driving forces and charge flows under the extremely spatially and temporally localized excitation. These results set the stage for versatile patterning and optical control over nanoscale currents in materials diagnostics, THz spectroscopies, nanomagnetism and ultrafast information processing.

36 MATERIALS SCIENCE↗

Observation of the axion quasiparticle in 2D MnBi 2 Te 4

The axion is a hypothetical fundamental particle that is conjectured to correspond to the coherent oscillation of the θ field in quantum chromodynamics. Its existence would solve multiple fundamental questions, including the strong CP problem of quantum chromodynamics and dark matter, but the axion has never been detected. Electrodynamics of condensed-matter systems can also give rise to a similar θ, so far studied as a static, quantized value to characterize the topology of materials. Coherent oscillation of θ in condensed matter has been proposed to lead to physics directly analogous to the high-energy axion particle—the dynamical axion quasiparticle (DAQ). Here we report the observation of the DAQ in MnBi 2 Te 4 . By combining a two-dimensional electronic device with ultrafast pump–probe optics, we observe a coherent oscillation of θ at about 44 gigahertz, which is uniquely induced by its out-of-phase antiferromagnetic magnon. This represents direct evidence for the presence of the DAQ, which in two-dimensional MnBi 2 Te 4 is found to arise from the magnon-induced coherent modulation of the Berry curvature. The DAQ also has implications in light–matter interaction and coherent antiferromagnetic spintronics, as it might lead to axion polaritons and electric control of ultrafast spin polarization. Finally, the DAQ could be used to detect axion particles. We estimate the detection frequency range and sensitivity in the millielectronvolt regime, which has so far been poorly explored.

topological matter↗

Photoinduced twist and untwist of moiré superlattices

This paper directly observes femtosecond photoinduced twist–untwist motion of WSe₂/MoSe₂ moiré superlattices using ultrafast electron diffraction, showing that optical excitation can dynamically reconfigure moiré lattice structure and interlayer coupling. It supports the proposal by establishing the team’s ability to probe ultrafast interfacial and moiré dynamics, which is relevant to using moiré TMDs as reconfigurable platforms for controlling spin, charge, and molecular interactions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Toward monochromated sub-nanometer UEM and femtosecond UED

A preliminary design of a mega-electron-volt (MeV) monochromator with 10 –5 energy spread for ultrafast electron diffraction (UED) and ultrafast electron microscopy (UEM) is presented. Such a narrow energy spread is advantageous in both the single shot mode, where the momentum resolution in diffraction is improved, and the accumulation mode, where shot-to-shot energy jitter is reduced. In the single-shot mode, we numerically optimized the monochromator efficiency up to 13% achieving 1.3 million electrons per pulse. In the accumulation mode, to mitigate the efficiency degradation caused by the shot-to-shot energy jitter, an optimized gun phase yields only a mild reduction of the single-shot efficiency, therefore the number of accumulated electrons nearly proportional to the repetition rate. Inspired by the recent work of Qi et al. (Phys Rev Lett 124:134803, 2020), a novel concept of applying reverse bending magnets to adjust the energy-dependent path length difference has been successfully realized in designing a MeV monochromator to achieve the minimum energy-dependent path length difference between cathode and sample. Thanks to the achromat design, the pulse length of the electron bunches and the energy-dependent timing jitter can be greatly reduced to the 10 fs level. The introduction of such a monochromator provides a major step forward, towards constructing a UEM with sub-nm resolution and a UED with ten-femtosecond temporal resolution. The one-to-one mapping between the electron beam parameter and the diffraction peak broadening enables a real-time nondestructive diagnosis of the beam energy spread and divergence. The tunable electric–magnetic monochromator allows the scanning of the electron beam energy with a 10 –5 precision, enabling online energy matching for the UEM, on-momentum flux maximizing for the UED and real-time energy measuring for energy-loss spectroscopy. A combination of the monochromator and a downstream chicane enables “two-color” double pulses with femtosecond duration and the tunable delay in the range of 10 to 160 fs, which can potentially provide an unprecedented femtosecond time resolution for time resolved UED.

36 MATERIALS SCIENCE↗

Extended X-ray absorption spectroscopy using an ultrashort pulse laboratory-scale laser-plasma accelerator

Laser-driven compact particle accelerators can provide ultrashort pulses of broadband X-rays, well suited for undertaking X-ray absorption spectroscopy measurements on a femtosecond timescale. Here the Extended X-ray Absorption Fine Structure (EXAFS) features of the K-edge of a copper sample have been observed over a 250 eV window in a single shot using a laser wakefield accelerator, providing information on both the electronic and ionic structure simultaneously. This capability will allow the investigation of ultrafast processes, and in particular, probing high-energy-density matter and physics far-from-equilibrium where the sample refresh rate is slow and shot number is limited. For example, states that replicate the tremendous pressures and temperatures of planetary bodies or the conditions inside nuclear fusion reactions. Using high-power lasers to pump these samples also has the advantage of being inherently synchronised to the laser-driven X-ray probe. A perspective on the additional strengths of a laboratory-based ultrafast X-ray absorption source is presented.

43 PARTICLE ACCELERATORS↗

Terahertz 2D coherent spectroscopy for probing and controlling multicorrelations in quantum matter

Terahertz 2D coherent spectroscopy (THz-2DCS) is an emerging technique that brings multidimensional resolution to the ultrafast spectral–temporal dynamics of non-equilibrium quantum phases of matter, enabling new capabilities for precise coherent control in many-body dynamics and multiorder correlations. Here, by mapping and disentangling complex excitation and detection pathways across distinct time and frequency dimensions, THz-2DCS provides a form of coherence tomography of light-induced quantum matter — revealing multiquantum coherences, separating nonlinear response functions and capturing collective modes and quantum kinetics on ultrafast THz timescales. This Perspective discusses the technical capabilities of THz-2DCS, provides a comparison to other multidimensional and coherent transient spectroscopies and looks ahead towards opportunities for advancing THz-2DCS instrumentation and experimental strategies towards new frontier discoveries.

Huang, Chuankun [Ames Laboratory (AMES), Ames, IA ↗

Dynamic signatures of spin-lattice coupling in the layered ferrimagnet Mn 3 Si 2 Te 6

Magnetic van der Waals (vdW) materials exhibit a profound interconnectedness between their various degrees of freedom, pointing to a wealth of potential applications in low-power and high-speed spintronic devices. Recently, light-matter interactions have been leveraged as robust, dynamic pathways to gain control over the properties of vdW magnets through the use of ultrafast pulses of light. Here, we utilize ultrafast photoexcitation to drive coherent lattice oscillations in the layered ferrimagnetic crystal Mn 3 Si 2 Te 6 , which significantly stiffen below the magnetic ordering temperature. We suggest that this is due to an exchange-mediated contraction of the lattice, stemming from strong magneto-structural coupling in this material. Furthermore, simulations of the transient incoherent response uncover the critical role of the spin-mediated electronic relaxation pathways. These results underscore the importance of spin-lattice coupling in vdW magnets and demonstrate a promising strategy for their dynamic optical control via their entangled degrees of freedom.

36 MATERIALS SCIENCE↗

A 3D nm-thin biomimetic membrane for ultimate molecular separation

Multi-functional membranes with high permeance and selectivity that can mimic nature's designs have tremendous industrial and bio-medical applications. In this paper, we report a novel concept of a 3D nanometer (nm)-thin membrane that can overcome the shortcomings of conventional membrane structures. Our 3D membrane is composed of two three-dimensionally interwoven channels that are separated by a continuous nm-thin amorphous TiO 2 layer. This 3D architecture dramatically increases the surface area by 6000 times, coupled with an ultra-short diffusion distance through the 2–4 nm-thin selective layer that allows for ultrafast gas and water transport, ~900 l m –2 h –1 bar –1 . The 3D membrane also exhibits a very high ion rejection (R ~ 100% for potassium ferricyanide) due to the combined size- and charge-based exclusion mechanisms. The combination of high ion rejection and ultrafast permeation makes our 3DM superior to the state-of-the-art high-flux membranes whose performances are limited by the flux-rejection tradeoff. Furthermore, its ultimate Li+ selectivity over polysulfide or gas can potentially solve major technical challenges in energy storage applications, such as lithium–sulfur or lithium–O 2 batteries.

36 MATERIALS SCIENCE↗

Toward Å-fs-meV Resolution in Electron Microscopy: Systematic Simulation of the Temporal Spread of Single-Electron Packets

Though efforts to improve the temporal resolution of transmission electron microscopes (TEMs) have waxed and waned for decades, with relatively recent advances routinely reaching sub-picosecond scales, fundamental and practical challenges have hindered the advance of combined Å-fs-meV resolutions, particularly for core-loss spectroscopy and real-space imaging. This is due in no small part to the complexity of the approach required to access timescales upon which electrons, atoms, molecules, and materials first begin to respond and transform – attoseconds to picoseconds. Here we present part of a larger effort devoted to systematically mapping the instrument parameter space of a TEM modified to reach ultrafast timescales. With General Particle Tracer, we studied the statistical temporal distributions of single-electron packets as a function of various fs pulsed-laser parameters and electron-gun configurations and fields for the exact architecture and dimensions of a Thermo Fisher Tecnai Femto ultrafast electron microscope. We focused on easily-adjustable parameters, such as laser pulse duration, laser spot size, photon energy, Wehnelt aperture diameter, and photocathode size. In addition to establishing trends and dispersion behaviors, we identify regimes within which packet duration can be 100s of fs and approach the 300-fs laser limit employed here. Overall, the results provide a detailed picture of the temporal behavior of single-electron packets in the Tecnai Femto gun region, forming the initial contribution of a larger effort.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗