The recently discovered phenomenon of broadband white-light emission at room temperature in the (110) two-dimensional organic-inorganic perovskite (N-MEDA)[PbBr4] (N-MEDA = N(1)-methylethane-1,2-diammonium) is promising for applications in solid-state lighting. However, the spectral broadening mechanism and, in particular, the processes and dynamics associated with the emissive species are still unclear. Herein, we apply a suite of ultrafast spectroscopic probes to measure the primary events directly following photoexcitation, which allows us to resolve the evolution of light-induced emissive states associated with white-light emission at femtosecond resolution. Terahertz spectra show fast free carrier trapping and transient absorption spectra show the formation of self-trapped excitons on femtosecond time-scales. Emission-wavelength-dependent dynamics of the self-trapped exciton luminescence are observed, indicative of an energy distribution of photogenerated emissive states in the perovskite. Our results are consistent with photogenerated carriers self-trapped in a deformable lattice due to strong electron-phonon coupling, where permanent lattice defects and correlated self-trapped states lend further inhomogeneity to the excited-state potential energy surface.

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

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.