Xijie Wang

Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

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.

Experimental demonstration of high quality MeV ultrafast electron diffraction.

The simulation optimization and an experimental demonstration of improved performances of mega-electron-volt ultrafast electron diffraction (MeV UED) are reported in this paper. Using ultrashort high quality electron pulses from an S-band photocathode rf gun and a polycrystalline aluminum foil as the sample, we experimentally demonstrated an improved spatial resolution of MeV UED, in which the Debye-Scherrer rings of the (111) and (200) planes were clearly resolved. This result showed that MeV UED is capable to achieve an atomic level spatial resolution and a approximately 100 fs temporal resolution simultaneously, and will be a unique tool for ultrafast structural dynamics studies.

Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

Absorption of light in hybrid perovskite solar cells leads to ultrafast large-amplitude deformations of the inorganic sublattice. Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb–I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier—lattice interactions, which fundamentally determine solar cell efficiencies.

Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses

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.

Dynamic Structural Response and Deformations of Monolayer MoS2 Visualized by Femtosecond Electron Diffraction

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.

Emittance studies of the BNL/SLAC/UCLA 1.6 cell photocathode RF gun

The symmetrized 1.6 cell S-band photocathode gun developed by the BNL/SLAC/UCLA collaboration is in operation at the Brookhaven Accelerator Test Facility (ATF). A novel emittance compensation solenoid magnet has also been designed, built and is in operation at the ATF. These two subsystems form an emittance compensated photoinjector used for beam dynamics, advanced acceleration and free electron laser experiments at the ATF. The highest acceleration field achieved on the copper cathode is 150 MV/m, and the guns normal operating field is 130 MV/m. The maximum rf pulse length is 3 /spl mu/s. The transverse emittance of the photoelectron beam were measured for various injection parameters. The 1 nC emittance results are presented along with electron bunch length measurements that indicated that at above the 400 pC, space charge bunch lengthening is occurring. The thermal emittance, /spl epsiv//sub 0/, of the copper cathode has been measured.

Observation of High Intensity X-Rays in Inverse Compton Scattering Experiment

Abstract We report the first results of high-intensity X-ray generation using Inverse Laser Compton scattering. This experiment was carried out by a US–Japan collaboration at the Brookhaven National Laboratory (BNL) Accelerator Test Facility (ATF) in September 1999. The 3.5 ps X-ray pulse at 6.5 keV, containing 3×10 6 X-ray photons was generated by the interaction of 60 MeV, 0.5 nC electron bunches and CO 2 laser pulses of 600 MW peak power.

Measurement of femtosecond electron pulse length and the temporal broadening due to space charge

The temporal width of ultrashort electron pulses as a function of beam intensity was measured on the femtosecond time scale with a customized streak camera. The results show that the temporal profile of an electron pulse is Gaussian at low beam intensity and progressively evolves to a top-hat shape due to space charge broadening as the beam intensity increases. The strong correlation between the pulse width and beam intensity observed in our streaking measurements agrees very well with the mean-field calculation and supports the main conclusion of previous theoretical studies that the space charge broadening plays a determinant role.

Interplay of the chirps and chirped pulse compression in a high-gain seeded free-electron laser

In a seeded high-gain free-electron laser (FEL), where a coherent laser pulse interacts with an ultrarelativistic electron beam, the seed laser pulse can be frequency chirped, and the electron beam can be energy chirped. Besides these two chirps, the FEL interaction introduces an intrinsic frequency chirp in the FEL even if the above-mentioned two chirps are absent. We examine the interplay of these three chirps. The problem is formulated as an initial value problem and solved via a Green function approach. Besides the chirp evolution, we also give analytical expressions for the pulse duration and bandwidth of the FEL, which remains fully longitudinally coherent in the high-gain exponential growth regime. Because the chirps are normally introduced for a final compression of the FEL pulse, some conceptual issues are discussed. We show that to get a short pulse duration, an energy chirp in the electron beam is important.

Efficiency enhancement using electron energy detuning in a laser seeded free electron laser amplifier

We report the experimental characterization of efficiency enhancement in a single-pass seeded free-electron laser (FEL) where the electron energy is detuned from resonance. Experiments show a doubling of the efficiency for beam energies above the resonant energy. Measurements of the FEL spectra versus energy detuning shows that the wavelength is governed by the seed laser. The variation in the gain length with beam energy was also observed. Good agreement is found between the experiment and numerical simulations using the MEDUSA simulation code.