We report the lattice dynamics of transition metal thin films by using the ultrafast electron diffraction. We observe a suppression of the diffraction intensity in a few picosecond after the photoexcitation, which is directly interpreted as the lattice heating via the electron-phonon interaction. The electron-phonon coupling constants for Au, Cu and Mo are quantitatively evaluated by employing the two-temperature model, which are consistent with those obtained by optical pump-probe methods. The variation in the lattice dynamics of the transition metals are systematically explained by the strength of the electron-phonon coupling, arising from the elemental dependence of the electronic structure and atomic mass.
We report on ultrafast electron diffraction on high quality single crystal silicon. The ultrafast dynamics of the Bragg peaks exhibits a giant photo-induced response which can only be explained in the framework of dynamical diffraction theory, taking into account multiple scattering of the probing electrons in the sample. In particular, we show that lattice heating following photo-excitation can cause an unexpected increase of the Bragg peak intensities, in contradiction with the well-known Debye-Waller effect. We anticipate that multiple scattering should be systematically considered in ultra…
Ultrafast lattice deformation of tens to hundreds of nanometer thick metallic crystals, after femtosecond laser excitation, was measured directly using 8.04 keV subpicosecond x-ray and 59 keV femtosecond electron pulses. Coherent phonons were generated in both single crystal and polycrystalline films. Lattice compression was observed within the first few picoseconds after laser irradiation in single crystal aluminum, which was attributed to the generation of a blast force and the propagation of elastic waves. The different time scale of lattice heating for tens and hundreds nanometer thick fil…
It has been technically challenging to concurrently probe the electrons and the lattices in materials during non-equilibrium processes, allowing their correlations to be determined. Here, in a single set of ultrafast electron diffraction patterns taken on the charge-density-wave (CDW) material 1T-TaSeTe, we discover a temporal shift in the diffraction intensity measurements as a function of scattering angle. With the help of dynamic models and theoretical calculations, we show that the ultrafast electrons probe both the valence-electron and lattice dynamic processes, resulting in the temporal …
Exciting electrons in solids with intense light pulses offers the possibility of generating new states of matter through nonthermal means and controlling their macroscopic properties on femto- to picosecond timescales. One way to manipulate a solid is by altering its lattice structure, which often underlies the electronic, magnetic and other phases. Here, we review how structures of solids are affected by photoexcitation and how their ultrafast dynamics are captured with time-resolved electron diffraction and microscopy. Specifically, we survey how a strong light pulse has been used to tailor …
One central challenge in understanding phonon thermal transport is a lack of experimental tools to investigate mode-based transport information. Although recent advances in computation lead to mode-based information, it is hindered by unknown defects in bulk region and at interfaces. Here we present a framework that can reveal microscopic phonon transport information in heterostructures, integrating state-of-the-art ultrafast electron diffraction (UED) with advanced scientific machine learning. Taking advantage of the dual temporal and reciprocal-space resolution in UED, we are able to reliabl…
Quantitative knowledge of electron-phonon coupling is important for many applications as well as for the fundamental understanding of nonequilibrium relaxation processes. Time-resolved diffraction provides direct access to this knowledge through its sensitivity to laser-induced lattice dynamics. Here, we present an approach for analyzing time-resolved polycrystalline diffraction data. A two-step routine is used to minimize the number of time-dependent fit parameters. The lattice dynamics are extracted by finding the best fit to the full transient diffraction pattern rather than by analyzing tr…
Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acou…
Metal-corroles are macrocycle organic molecules with numerous practical applications. In particular, copper corroles exhibit an interesting saddled geometry, which has attracted significant attention from theoreticians and experimentalists over the years. The present work is dedicated to understand the effect of structural saddling in a copper corrole on potential probe signals via imaging ultrafast coherent electron dynamics. A linearly polarized pulse is used to trigger the electron dynamics and time-resolved x-ray diffraction is employed to image the triggered dynamics. It is found that the…
Dynamical diffraction effects in single crystals produce highly monochromatic parallel X-ray beams with a mutual separation of a few micrometer and a time-delay of a few fs -the so-called echoes. This ultrafast diffraction effect is used at X-ray Free Electron Lasers in self-seeding schemes to improve beam monochromaticity. Here, we present a coherent X-ray imaging measurement of echoes from Si crystals and demonstrate that a small surface strain can be used to tune their temporal delay. These results represent a first step towards the ambitious goal of strain-tailoring new X-ray optics.
We introduce ultrafast low-energy electron diffraction (ULEED) in backscattering for the study of structural dynamics at surfaces. Using a tip-based source of ultrashort electron pulses, we investigate the optically-driven transition between charge-density wave phases at the surface of 1T-TaS2. The large transfer width of the instrument allows us to employ spot-profile analysis, resolving the phase-ordering kinetics in the nascent incommensurate charge-density wave phase. We observe a coarsening that follows a power-law scaling of the correlation length, driven by the annihilation of dislocati…
Band bending at semiconductor surfaces induced by chemical doping or electric fields can create metallic surfaces with properties not found in the bulk, such as high electron mobility, magnetism or superconductivity. Optical generation of such metallic surfaces via BB on ultrafast timescales would facilitate a drastic manipulation of the conduction, magnetic and optical properties of semiconductors for high-speed electronics. Here, we demonstrate the ultrafast generation of a metal at the (10-10) surface of ZnO upon photoexcitation. Compared to hitherto known ultrafast photoinduced semiconduct…
As a 3D topological insulator, bismuth selenide (Bi2Se3) has potential applications for electrically and optically controllable magnetic and optoelectronic devices. How the carriers interact with lattice is important to understand the coupling with its topological phase. It is essential to measure with a time scale smaller than picoseconds for initial interaction. Here we use an X-ray free-electron laser to perform time-resolved diffraction to study ultrafast carrier-induced lattice contractions and interlayer modulations in Bi2Se3 thin films. The lattice contraction depends on the carrier con…
Bulk layered MX2 transition metal chalcogenides (M = Mo, W and X = S, Se) are known to exhibit an indirect to direct band gap transition as the number of layers is reduced. Previous time-resolved work has principally focused on the investigation of the transient evolution of the band structure after photo-excitation, but additional information on the dynamics of the concomitant lattice rearrangement is needed to fully understand this phenomenon. Here, ultrafast electron diffraction is used to probe the atomic motion and bond dilation in monolayer WSe2 with femtosecond temporal resolution. The …
Femtosecond carrier recombination in PbI2 is measured using tabletop high-harmonic extreme ultraviolet (XUV) transient absorption spectroscopy and ultrafast electron diffraction. XUV absorption from 45 eV to 62 eV measures transitions from the iodine 4d core level to the conduction band density of states. Photoexcitation at 400 nm creates separate and distinct transient absorption signals for holes and electrons, separated in energy by the 2.4 eV band gap of the semiconductor. The shape of the conduction band and therefore the XUV absorption spectrum is temperature dependent, and nonradiative …
The ultrafast dynamics of the octahedral rotation in Ca:SrTiO3 is studied by time resolved x-ray diffraction after photo excitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO3, we observe a ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperaure despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on…
Time-resolved x-ray diffraction has been used to measure the low-temperature thermal transport properties of a Pt/Gd3Fe5O12//Gd3Ga5O12 metal/oxide heterostructure relevant to applications in spin caloritronics. A pulsed femtosecond optical signal produces a rapid temperature rise in the Pt layer, followed by heat transport into the Gd3Fe5O12 (GdIG) thin film and the Gd3Ga5O12 (GGG) substrate. The time dependence of x-ray diffraction from the GdIG layer was tracked using an accelerator-based femtosecond x-ray source. The ultrafast diffraction measurements probed the intensity of the GdIG (1 -1 …
Understanding ultrafast x-ray 'echoes' diffracted from single crystals
European XFEL Facility GmbH（欧洲X射线自由电子激光设施有限公司）；Diamond Light Source（钻石光源）；ESRF（欧洲同步辐射装置）；MAX IV Laboratory, Lund University（隆德大学马克四实验室）；PSI Center for Photon Science, Paul Scherrer Institute（保罗谢勒研究所光子科学中心）
We predict ultrafast modulation of the pure molten metal surface stress fields under the irradiation of the single femtosecond laser pulse through the two-temperature model molecular-dynamics simulations. High-resolution and precision calculations are used to resolve the ultrafast laser-induced anisotropic relaxations of the pressure components on the time-scale comparable to the intrinsic liquid density relaxation time. The magnitudes of the dynamic surface tensions are found being modulated sharply within picoseconds after the irradiation, due to the development of the nanometer scale non-hy…
We study the transient photoluminescence (PL) of photoexcited metals by solving the Boltzmann equation considering the effects of electron-electron (e-e) and electron-phonon (e-ph) collisions, where the e-ph coupling function is calculated from first-principles in order to account for the energy transfer rate between electrons and phonons accurately. We apply the present scheme to the transient PL of silver and demonstrate that the agreement between the theory and experiment is good, where the effect of nonequilibrium electron distribution is significant to fit the experimental data. The effec…
Enabling the light-control of complex systems on ultra-short timescales gives rise to rich physics with promising applications. While crucial, the quantitative determination of both the longitudinal and shear photo-induced strains still remains challenging. Here, by scrutinizing asymmetric Bragg peaks pairs $(\pm h01)$ using picosecond time-resolved X-ray diffraction experiments in BiFeO$_3$, we simultaneously determine the longitudinal and shear strains. The relative amplitude of those strains can be explained only if both thermal and non-thermal processes contribute to the acoustic phonon ph…
Strongly correlated materials that exhibit an insulator-metal transition are key candidates in the search for new computing platforms. Understanding the pathways and timescales underlying the electrically-driven insulator-metal transition is crucial for uncovering the fundamental limits of device operation. Using stroboscopic electron diffraction, we perform synchronized time-resolved measurements of atomic motions and electronic transport in operating vanadium dioxide switches. We discover an electrically-triggered, isostructural state that forms transiently on microsecond timescales, stabili…
We present a combined ultrafast optical pump-probe and ultrafast x-ray diffraction measurement of the CDW dynamics in SmTe$_3$ at 300 K. The ultrafast x-ray diffraction measurements, taken at the Linac Coherent Light Source reveal a $\sim 1.55$ THz mode that becomes overdamped with increasing fluence. We identify this oscillation with the lattice component of the amplitude mode. Furthermore, these data allow for a more clear identification of the frequencies present in the optical pump-probe data. In both, reflectivity and diffraction, we observe a crossover of the response from linear (for sm…
Impacts of Hot Electron Diffusion, Electron-Phonon Coupling, and Surface Atoms on Metal Surface Dynamics Revealed by Reflection Ultrafast Electron Diffraction
Time-domain femtosecond laser spectroscopic measurements of the ultrafast lattice dynamics in 2H-MoTe2 bulk crystals were carried out to understand the carrier-phonon interactions that govern electronic transport properties. An unusually long lifetime coherent A1g phonon mode was observed even in the presence of very large density of photo-excited carriers at room temperature. The decay rate was observed to decrease with increasing excitation laser fluence. Based on the laser fluence dependence including the inducement of significant phonon softening and a peculiar decrease in phonon decay rat…
Atomic rearrangements within crystals lie at the foundation of electron-phonon-coupled phenomena such as metal-insulator transition and superconductivity. Advanced laser-pump-probe studies have recently focused on various charge-density-wave (CDW) materials to sharpen our understanding of the charge-lattice entanglement, where non-thermal melting of the CDW state is evident from the enhanced Bragg diffraction peak intensities - attributed to the dominance of the metal-atom dynamics over the nonmetal-anion one. Here using ultrafast MeV electron diffraction on the prototypical CDW material 1T-Ta…
We use femtosecond electron diffraction to study ultrafast lattice dynamics in the highly correlated antiferromagnetic (AF) semiconductor NiO. Using the scattering vector (Q) dependence of Bragg diffraction, we introduce a Q-resolved effective lattice temperature, and identify a nonthermal lattice state with preferential displacement of O compared to Ni ions, which occurs within ~0.3 ps and persists for 25 ps. We associate this with transient changes to the AF exchange striction-induced lattice distortion, supported by the observation of a transient Q-asymmetry of Friedel pairs. Our observatio…
Since the discovery of electron-wave duality, electron scattering instrumentation has developed into a powerful array of techniques for revealing the atomic structure of matter. Beyond detecting local lattice variations in equilibrium structures, recent research efforts have been directed towards the long sought-after dream of visualizing the dynamic evolution of matter in real-time. The atomic behavior at ultrafast timescales carries critical information on phase transition and chemical reaction dynamics, the coupling of electronic and nuclear degrees of freedom in materials and molecules, th…
In ultrafast electron diffraction (UED) experiments, accurate retrieval of time-resolved structural parameters, such as atomic coordinates and thermal displacement parameters, requires an accurate scattering model. Unfortunately, kinematical models are often inaccurate even for relativistic electron probes, especially for dense, oriented single crystals where strong channeling and multiple scattering effects are present. This article introduces and demonstrates dynamical scattering models tailored for quantitative analysis of UED experiments performed on single-crystal films. As a case study, …
We demonstrate that highly-ordered two-dimensional crystals of ligand-capped gold nanoparticles display a local photo-mechanical stiffness as high as that of solids such as graphite. In out-of equilibrium electron diffraction experiments, a strong temperature jump is induced in a thin film with a femtosecond laser pulse. The initial electronic excitation transfers energy to the underlying structural degrees of freedom, with a rate generally proportional to the stiffness of the material. With femtosecond small-angle electron diffraction, we observe the temporal evolution of the diffraction feat…
