arXiv subjects

C. A. Pennington

Publications and source records attributed to C. A. Pennington.

5 recordsLinked to original sources

arXiv2025

Photoinduced twist and untwist of moiré superlattices in TMDC heterobilayers

Two-dimensional moiré materials are formed by artificially stacking atomically thin monolayers. A wealth of correlated and topological quantum phases can be engineered via precise choice of stacking geometry. These designer electronic properties depend crucially on interlayer coupling and atomic registry. An important open question is how atomic registry responds on ultrafast timescales to optical excitation and whether the moiré geometry can be dynamically reconfigured to tune emergent phenomena in real time. Here we show that femtosecond photoexcitation drives a coherent twist-untwist motion of the moiré superlattice in $2^\circ$ and $57^\circ$ twisted WSe$_2$/MoSe$_2$ heterobilayers, resolved directly by ultrafast electron diffraction. Upon above-band-gap photoexcitation, the moiré superlattice diffraction features are enhanced within 1 ps and subsequently suppressed several picoseconds after, deviating markedly from typical photoinduced lattice heating. Kinetic diffraction analysis, supported by simulations of the sample dynamics, indicates a peak-to-trough local twist angle modulation of $0.6^\circ$, correlated with a sub-THz frequency moiré phonon. This motion is driven by ultrafast charge transfer that transiently increases interlayer attraction. Our results could lead to ultrafast control of moiré periodic lattice distortions and, by extension, the local moiré potential that shapes excitons, polarons, and correlation-driven behaviors

cond-mat.mtrl-sci↗

arXiv2023

Multi-scale time-resolved electron diffraction: A case study in moiré materials

Ultrafast-optical-pump -- structural-probe measurements, including ultrafast electron and x-ray scattering, provide direct experimental access to the fundamental timescales of atomic motion, and are thus foundational techniques for studying matter out of equilibrium. High-performance detectors are needed in scattering experiments to obtain maximum scientific value from every probe particle. We deploy a hybrid pixel array direct electron detector to perform ultrafast electron diffraction experiments on a WSe$_2$/MoSe$_2$ 2D heterobilayer, resolving the weak features of diffuse scattering and moiré superlattice structure without saturating the zero order peak. Enabled by the detector's high frame rate, we show that a chopping technique provides diffraction difference images with signal-to-noise at the shot noise limit. Finally, we demonstrate that a fast detector frame rate coupled with a high repetition rate probe can provide continuous time resolution from femtoseconds to seconds, enabling us to perform a scanning ultrafast electron diffraction experiment that maps thermal transport in WSe$_2$/MoSe$_2$ and resolves distinct diffusion mechanisms in space and time.

physics.ins-det↗

arXiv2023

Atomically smooth films of CsSb: a chemically robust visible light photocathode

Alkali antimonide semiconductor photocathodes provide a promising platform for the generation of high brightness electron beams, which are necessary for the development of cutting-edge probes including x-ray free electron lasers and ultrafast electron diffraction. However, to harness the intrinsic brightness limits in these compounds, extrinsic degrading factors, including surface roughness and contamination, must be overcome. By exploring the growth of CsxSb thin films monitored by in situ electron diffraction, the conditions to reproducibly synthesize atomically smooth films of CsSb on 3C-SiC (100) and graphene coated TiO2 (110) substrates are identified, and detailed structural, morphological, and electronic characterization is presented. These films combine high quantum efficiency in the visible (up to 1.2% at 400 nm), an easily accessible photoemission threshold of 550 nm, low surface roughness (down to 600 pm on a 1 um scale), and a robustness against oxidation up to 15 times greater then Cs3Sb. These properties suggest that CsSb has the potential to operate as an alternative to Cs$_3$Sb in electron source applications where the demands of the vacuum environment might otherwise preclude the use of traditional alkali antimonides.

physics.acc-ph↗

arXiv2022

Four-Dimensional Emittance Measurements of Ultrafast Electron Diffraction Optics Corrected Up to Sextupole Order

Ultrafast electron diffraction (UED) is a technique in which short-pulse electron beams can probe the femtosecond-scale evolution of atomic structure in matter driven far from equilibrium. As an accelerator physics challenge, UED imposes stringent constraints on the brightness of the probe electron beam. The low normalized emittance employed in UED, often at the 10 nm scale and below, is particularly sensitive to both applied field aberrations and space charge effects. The role of aberrations is increasingly important in small probe systems that often feature multiple orders of magnitude variations in beam size during transport. In this work, we report the correction of normal quadrupole, skew quadrupole, and sextupole aberrations via dedicated corrector elements in an ultrafast electron micro-diffraction beamline. To do this, we generate precise 4-dimensional phase space maps of rf-compressed electron beams, and find excellent agreement with aberration-free space charge simulations. Finally, we discuss the role a probe-forming aperture can play in improving the brightness of bunches with appreciable space charge effects.

physics.acc-ph↗

arXiv2022

A kiloelectron-volt ultrafast electron micro-diffraction apparatus using low emittance semiconductor photocathodes

We report the design and performance of a time-resolved electron diffraction apparatus capable of producing intense bunches with simultaneously single digit micron probe size, long coherence length, and $200$ fs rms time resolution. We measure the 5d (peak) beam brightness at the sample location in micro-diffraction mode to be $7 \times 10^{13} \ \mathrm{A}/\text{m}^2\text{-rad}^2$. To generate high brightness electron bunches, the system employs high efficiency, low emittance semiconductor photocathodes driven with a wavelength near the photoemission threshold at a repetition rate up to 250 kHz. We characterize spatial, temporal, and reciprocal space resolution of the apparatus. We perform proof-of-principle measurements of ultrafast heating in single crystal Au samples and compare experimental results with simulations that account for the effects of multiple-scattering.

physics.acc-ph↗