Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability. C 2015 AIP Publishing LLC. [http://dx

Two-dimensional materials are subject to intrinsic and dynamic rippling that modulates their optoelectronic and electromechanical properties. Here, we directly visualize the dynamics of these processes within monolayer transition metal dichalcogenide MoS2 using femtosecond electron scattering techniques as a real-time probe with atomic-scale resolution. We show that optical excitation induces large-amplitude in-plane displacements and ultrafast wrinkling of the monolayer on nanometer length-scales, developing on picosecond time-scales. These deformations are associated with several percent peak strains that are fully reversible over tens of millions of cycles. Direct measurements of electron-phonon coupling times and the subsequent interfacial thermal heat flow between the monolayer and substrate are also obtained. These measurements, coupled with first-principles modeling, provide a new understanding of the dynamic structural processes that underlie the functionality of two-dimensional materials and open up new opportunities for ultrafast strain engineering using all-optical methods.

Observing the motion of the nuclear wavepackets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wavepacket in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 Å and temporal resolution of 230 fs full-width at half-maximum (FWHM). The method is not only sensitive to the position but also the shape of the nuclear wavepacket.Photo-induced reactions are of particular interest for understanding the fundamental mechanisms driving the conversion of light into chemical and kinetic energy on ultrafast time scales. The coherent nuclear motion is particularly important to study the reaction pathway and energy conversion efficiency in processes that cannot be described using the Born-Oppenheimer approximation. Diffraction-based techniques, such as ultrafast electron and x-ray diffraction offer a unique advantage for imaging the molecular geometry as those measurements are directly sensitive to the spatial distribution of atoms, and are thus complementary to spectroscopic methods that are sensitive to energy differences between electronic states. The nuclear motion in

Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angström spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 Å) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.

We use ultrafast electron diffraction to detect the temporal evolution of phonon populations in femtosecond laser-excited ultrathin single-crystalline gold films. From the time-dependence of the Debye-Waller factor we extract a 4.7 ps timeconstant for the increase in mean-square atomic displacements. We show from the increase of the diffuse scattering intensity that the population of phonon modes near the X and K points in the Au fcc Brillouin zone grows with timescales of 2.3 and 2.9 ps, respectively, faster than the Debye-Waller average. We find that thermalization continues within the initially nonequilibrium phonon distribution after 10 ps. The observed momentum dependent timescale of phonon populations is in contrast to what is usually predicted in a two-temperature model.

Magnetostriction, the strain induced by a change in magnetization, is a universal effect in magnetic materials. Owing to the difficulty in unraveling its microscopic origin, it has been largely treated phenomenologically. Here, we show how the source of magnetostriction—the underlying magnetoelastic stress—can be separated in the time domain, opening the door for an atomistic understanding. X-ray and electron diffraction are used to separate the sub-picosecond spin and lattice responses of FePt nanoparticles. Following excitation with a 50-fs laser pulse, time-resolved X-ray diffraction demonstrates that magnetic order is lost within the nanoparticles with a time constant of 146 fs. Ultrafast electron diffraction reveals that this demagnetization is followed by an anisotropic, three-dimensional lattice motion. Analysis of the size, speed, and symmetry of the lattice motion, together with ab initio calculations accounting for the stresses due to electrons and phonons, allow us to reveal the magnetoelastic stress generated by demagnetization.

Alkali-antimonide photocathodes were grown on Si(100) and studied by means of XPS and UHV-AFM to validate the growth procedure and morphology of this material. The elements were evaporated sequentially at elevated substrate temperatures (first Sb, second K, third Cs). The generated intermediate K-Sb compound itself is a photocathode and the composition of K2.4Sb is close to the favored K3Sb stoichiometry. After cesium deposition, the surface layer is cesium enriched. The determined rms roughness of 25 nm results in a roughness domination of the emittance in the photoinjector already above 3 MV/m

Free-electron lasers and energy recovery linacs represent a new generation of ultra-high brightness electron accelerator based x-ray sources. Photocathodes are a critical performance-limiting component of these systems. Here, we describe the development of photocathodes based on potassium-cesium-antimonide that satisfy many of the key requirements of future light sources, such as robustness, high quantum efficiency when excited with visible light, and low transverse emittance.