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

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 Coherent Nuclear Motion in Isolated Molecules.

Observing the motion of the nuclear wave packets 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 wave packet 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. The method is not only sensitive to the position but also the shape of the nuclear wave packet.

Femtosecond gas phase electron diffraction with MeV electrons.

We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution.

Demonstration of acceleration of relativistic electrons at a dielectric microstructure using femtosecond laser pulses.

Acceleration of electrons using laser-driven dielectric microstructures is a promising technology for the miniaturization of particle accelerators. Achieving the desired GV m-1 accelerating gradients is possible only with laser pulse durations shorter than ∼1 ps. In this Letter, we present, to the best of our knowledge, the first demonstration of acceleration of relativistic electrons at a dielectric microstructure driven by femtosecond duration laser pulses. Using this technique, an electron accelerating gradient of 690±100 MV m-1 was measured-a record for dielectric laser accelerators.

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.

Electron beam position monitor for a dielectric microaccelerator.

We report the fabrication and first demonstration of an electron beam position monitor for a dielectric microaccelerator. This device is fabricated on a fused silica substrate using standard optical lithography techniques and uses the radiated optical wavelength to measure the electron beam position with a resolution of 10 µm, or 7% of the electron beam spot size. This device also measures the electron beam spot size in one dimension.

Band-gap guidance in optically induced photonic lattices with a negative defect.

We report the first experimental demonstration of band-gap guidance of light in an optically induced two-dimensional photonic lattice with a single-site negative defect (akin to a low-index core in photonic-crystal fibers). We discuss the difference between spatial guidance at a regular and a defect site, and show that the guided beam through the defect displays fine structures such as vortex cells that arise from defect modes excited at higher band gaps. Defect modes at different wavelengths are also observed.

Observation of two-dimensional lattice vector solitons.

We demonstrate the formation of fundamental and dipolelike vector solitons in an optically induced two-dimensional photonic lattice. Such vector solitons are realized by mutual trapping of two beams in the lattice. Our theoretical results are in good agreement with experimental observations.

Dipole solitons in optically induced two-dimensional photonic lattices.

Dipole solitons in a two-dimensional optically induced photonic lattice are theoretically predicted and experimentally demonstrated for the first time to our knowledge. It is shown that such dipole solitons are stable and robust under appropriate conditions. Our experimental results are in good agreement with theoretical predictions.

Observation of discrete vortex solitons in optically induced photonic lattices.

We report on the first experimental observation of discrete vortex solitons in two-dimensional optically induced photonic lattices. We demonstrate strong stabilization of an optical vortex by the lattice in a self-focusing nonlinear medium and study the generation of the discrete vortices from a broad class of singular beams.