arXiv subjects

S. Weathersby

Publications and source records attributed to S. Weathersby.

7 recordsLinked to original sources

arXiv2025

Imaging the Photochemistry of Cyclobutanone using Ultrafast Electron Diffraction: Experimental Results

We investigated the ultrafast structural dynamics of cyclobutanone following photoexcitation at $\lambda=200$ nm using gas-phase megaelectronvolt ultrafast electron diffraction. Our investigation complements the simulation studies of the same process within this special issue. It provides information about both electronic state population and structural dynamics through well-separable inelastic and elastic electron scattering signatures. We observe the depopulation of the photoexcited S$_2$ state of cyclobutanone with n3s Rydberg character through its inelastic electron scattering signature with a time constant of $(0.29 \pm 0.2)$ ps towards the S$_1$ state. The S$_1$ state population undergoes ring-opening via a Norrish Type-I reaction, likely while passing through a conical intersection with S$_0$. The corresponding structural changes can be tracked by elastic electron scattering signatures. These changes appear with a delay of $(0.14 \pm 0.05)$ ps with respect the initial photoexcitation, which is less than the S$_2$ depopulation time constant. This behavior provides evidence for the ballistic nature of the ring-opening once the S$_1$ state is reached. The resulting biradical species react further within $(1.2 \pm 0.2)$ ps via two rival fragmentation channels yielding ketene and ethylene, or propene and carbon monoxide. Our study showcases both the value of gas-phase ultrafast diffraction studies as an experimental benchmark for nonadiabatic dynamics simulation methods and the limits in the interpretation of such experimental data without comparison to such simulations.

physics.chem-ph↗

arXiv2021

Effect of lattice excitations on transient near edge X-ray absorption spectroscopy

Time-dependent and constituent-specific spectral changes in soft near edge X-ray spectroscopy (XAS) of an [Fe/MgO]$_8$ metal/insulator heterostructure upon laser excitation are analyzed at the O K-edge with picosecond time resolution. The oxygen absorption edge of the insulator features a uniform intensity decrease of the fine structure at elevated phononic temperatures, which can be quantified by a simple simulation and fitting procedure presented here. Combining X-ray absorption spectroscopy with ultrafast electron diffraction measurements and ab initio calculations demonstrate that the transient intensity changes in XAS can be assigned to a transient lattice temperature. Thus, the sensitivity of transient near edge XAS to phonons is demonstrated.

cond-mat.mtrl-sci↗

arXiv2019

SLAC UED LLRF System Upgrade

The SLAC mega-electron-volt (MeV) ultrafast electron diffraction (UED) instrument is a powerful "electron camera" for the study of time-resolved, ultrafast atomic & molecular dynamics in chemical and solid-state systems. The UED laser timing synchronization is upgraded to SLAC (Advanced Telecommunications Computing Architecture) ATCA based femtosecond laser timing synchronization system. UED radio frequency (RF) gun cavity low level RF (LLRF) control is also being upgraded to SLAC ATCA based LLRF system to provide improved performance and maintainability. The new laser timing synchronization and LLRF control are implemented in one ATCA crate located in the laser room. A 2nd ATCA crate is set up to monitor the Klystron and sub-booster performance. With the ATCA based RF control system, the laser timing jitter has achieved 10 fs. The UED operation beam rate is being upgraded from 180 Hz to 360 Hz, which paves the way for a further upgrade of operation beam rate to 1 kHz in the future. In this paper, we present design details and characterization results of the implementation.

physics.acc-ph↗

arXiv2019

Microscopic non-equilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure

The element specificity of soft X-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. Using [Fe/MgO]$_n$ as a model system, we perform ultraviolet pump/soft X-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield comprehensive insight into the microscopic processes leading to local relaxation within a single constituent or non-local relaxation between two constituents. Besides electronic excitations in Fe, which are monitored at the Fe L$_3$ absorption edge and relax within 1 ps by electron-phonon coupling, soft X-ray analysis identifies a change at the oxygen K absorption edge of the MgO layers which occurs within 0.5 ps. This ultrafast energy transfer across the Fe-MgO interface is mediated by high-frequency, interface vibrational modes, which are excited by hot electrons in Fe and couple to vibrations in MgO in a mode-selective, non-thermal manner. A second, slower timescale is identified at the oxygen K pre-edge and the Fe L$_3$ edge. The slower process represents energy transfer by acoustic phonons and contributes to thermalization of the entire heterostructure. We thus find that the interfacial energy transfer is associated with non-equilibrium behavior in the phonon system. Because our experiments lack signatures of charge transfer across the interface, we conclude that phonon-mediated processes dominate the competition of electronic and lattice excitations in these non-local, non-equilibrium dynamics.

cond-mat.mtrl-sci↗

arXiv2019

Nanopatterned electron beams for temporal coherence and deterministic phase control of x-ray free-electron lasers

We demonstrate the ability to create electron beams with high-contrast, nanometer-scale density modulations as a first step toward developing full control of the phase fronts of an x-ray free-electron laser. The nanopatterned electron beams are produced by diffracting electrons through thin single-crystal silicon membranes that are lithographically patterned to different thicknesses. For transform-limited x-ray production the desired pattern is a series of regularly spaced lines (i.e. a grating) that generate uniformly spaced nanobunches of electrons, however nearly any pattern can be etched in the silicon, such as frequency-chirps or multiple patterns of different colors or line spacings. When these patterns are transferred from the spatial to the temporal dimension by accelerator electromagnetic optics they will control the phase fronts of coherent x-rays, giving unprecedented deterministic control over the phase of ultrashort x-ray pulses. In short, this method allows the time-structure for a fully coherent x-ray beam to be generated from a pattern written on a semiconductor wafer by lithography.

physics.acc-ph↗

arXiv2019

Theoretical and experimental electron diffraction intensity maps for single crystal silicon from an ultrafast source

Electron diffraction through a thin patterned silicon membrane can be used to create complex spatial modulations in electron distributions by varying the intensity of different reflections using parameters such as crystallographic orientation and wafer thickness, then selecting specific spots in the diffraction plane using apertures. The patterned electron beams can be used to control phase and amplitude of subsequent x-ray emission, enabling novel coherent x-ray methods. The electrons themselves can also be used for femtosecond time resolved diffraction and microscopy. As a first step toward patterned beams, we demonstrate experimentally and through simulation the ability to accurately predict and control diffraction spot intensities. We simulate MeV transmission electron diffraction patterns using the multislice method for various crystallographic orientations of a single crystal Si(100) membrane near beam normal. The resulting intensity maps of the Bragg reflections are compared to experimental results obtained at the Accelerator Structure Test Area Ultrafast Electron Diffraction (ASTA UED) facility at SLAC. Furthermore, the fraction of inelastic and elastic scattering of the initial charge is estimated along with the absorption of the membrane to determine the contrast that would be seen in a patterned version of the Si(100) membrane.

physics.acc-ph↗

arXiv2011

Status of the Super-B factory Design

The SuperB international team continues to optimize the design of an electron-positron collider, which will allow the enhanced study of the origins of flavor physics. The project combines the best features of a linear collider (high single-collision luminosity) and a storage-ring collider (high repetition rate), bringing together all accelerator physics aspects to make a very high luminosity of 10$^{36}$ cm$^{-2}$ sec$^{-1}$. This asymmetric-energy collider with a polarized electron beam will produce hundreds of millions of B-mesons at the $Υ$(4S) resonance. The present design is based on extremely low emittance beams colliding at a large Piwinski angle to allow very low $β_y^\star$ without the need for ultra short bunches. Use of crab-waist sextupoles will enhance the luminosity, suppressing dangerous resonances and allowing for a higher beam-beam parameter. The project has flexible beam parameters, improved dynamic aperture, and spin-rotators in the Low Energy Ring for longitudinal polarization of the electron beam at the Interaction Point. Optimized for best colliding-beam performance, the facility may also provide high-brightness photon beams for synchrotron radiation applications.

physics.acc-ph↗