Jeff Corbett

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.

Mechanism for Broadband White-Light Emission from Two-Dimensional (110) Hybrid Perovskites

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.

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 0.07xa0Å and temporal resolution of 230xa0fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.

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 100u2009fs root-mean-squared temporal resolution and sub-Angstrom (0.76u2009Å) 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 300u2009fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.

Accelerator control middle layer

This paper reviews an efficient implementation of the software middle layer that resides between high-level accelerator control applications and the low-level accelerator control system. The middle layer software is written in MATLAB and includes links to the EPICS Channel Access Library. Functionally, the middle layer syntax closely parallels the Family/Index naming scheme used in many accelerator simulation codes and uses the same convention to communicate with both the online machine and the accelerator model. Hence, machine control, machine simulation and data analysis tools are integrated into a single, easy-to-use software package.

Low alpha mode for SPEAR3

In the interest of obtaining shorter bunch length for shorter X-ray pulses, we have developed a low-alpha operational mode for SPEAR3. In this mode the momentum compaction factor is reduced by a factor of 21 or more from the usual achromat mode by introducing negative dispersion at the straight sections. We successfully stored 100 mA with the normal fill pattern at a lifetime of 30 hrs. The bunch length was measured to be 6.9 ps, compared to 17 ps in the normal mode. In this paper we report our studies on the lattice design and calibration, orbit stability, higher order alpha measurement, lifetime measurement and its dependence on the sextupoles, injection efficiency, longitudinal stability and bunch lengths.

An Accelerator Control Middle Layer Using Matlab

Matlab is an interpretive programming language originally developed for convenient use with the LINPACK and EISPACK libraries. Matlab is appealing for accelerator physics because it is matrix-oriented, provides an active workspace for system variables, powerful graphics capabilities, built-in math libraries, and platform independence. A number of accelerator software toolboxes have been written in Matlab - the Accelerator Toolbox (AT) for model-based machine simulations, LOCO for on-line model calibration, and Matlab Channel Access (MCA) to connect with EPICS. The function of the MATLAB ‘Middle Layer’ is to provide a scripting language for machine simulations and on-line control, including non-EPICS based control systems. The Middle Layer has simplified and streamlined development of high-level applications including configuration control, energy ramp, orbit correction, photon beam steering, ID compensation, beam-based alignment, tune correction and response matrix measurement. The database-driven Middle Layer software is largely machine-independent and easy to port. Six accelerators presently use the software package with more scheduled to come on line soon.

Measurement of transient atomic displacements in thin films with picosecond and femtometer resolution.

We report measurements of the transient structural response of weakly photo-excited thin films of BiFeO3, Pb(Zr,Ti)O3, and Bi and time-scales for interfacial thermal transport. Utilizing picosecond x-ray diffraction at a 1.28u2009MHz repetition rate with time resolution extending down to 15u2009ps, transient changes in the diffraction angle are recorded. These changes are associated with photo-induced lattice strains within nanolayer thin films, resolved at the part-per-million level, corresponding to a shift in the scattering angle three orders of magnitude smaller than the rocking curve width and changes in the interlayer lattice spacing of fractions of a femtometer. The combination of high brightness, repetition rate, and stability of the synchrotron, in conjunction with high time resolution, represents a novel means to probe atomic-scale, near-equilibrium dynamics.

Thickness-dependent electron–lattice equilibration in laser-excited thin bismuth films

Electron–phonon coupling processes determine electronic transport properties of materials and are responsible for the transfer of electronic excess energy to the lattice. With decreasing device dimensions an understanding of these processes in nanoscale materials is becoming increasingly important. Here we use time-resolved electron diffraction to directly study energy relaxation in thin bismuth films after optical excitation. Precise measurements of the transient Debye–Waller-effect for various film thicknesses and over an extended range of excitation fluences allow to separate different contributions to the incoherent lattice response. While phonon softening in the electronically excited state is responsible for an immediate increase of the r.m.s. atomic displacement within a few hundred fs, ordinary electron–phonon coupling leads to subsequent heating of the material on a few ps time-scale. The data reveal distinct changes in the energy transfer dynamics which becomes faster for stronger excitation and smaller film thickness, respectively. The latter effect is attributed to a cross-interfacial coupling of excited electrons to phonons in the substrate.

Experimental verification of the 3-step model of photoemission for energy spread and emittance measurements of copper and CsBr-coated copper photocathodes suitable for free electron laser applications

This paper presents measurements and analysis of the quantum efficiency (QE) and intrinsic emittance of Cu and CsBr coated Cu photocathodes. The data analysis uses expressions for the quantum efficiency and the intrinsic emittance for metal cathodes previously derived from Spicers three-step model of photoemission. Data taken with a 257u2009nm CW laser on (100) Cu crystals indicate an emittance of 0.77 (μm/mm-rms) for CsBr coated and 0.42 (μm/mm-rms) for uncoated cathodes. The high quantum efficiency and low emittance observed for CsBr coated cathodes have applications in free electron laser and other devices requiring high brightness electron beams.