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Results for “ULTRAFAST ELECTRON DIFFRACTION”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Multi-objective Bayesian active learning for MeV-ultrafast electron diffraction

Ultrafast electron diffraction using MeV energy beams(MeV-UED) has enabled unprecedented scientific opportunities in the study of ultrafast structural dynamics in a variety of gas, liquid and solid state systems. Broad scientific applications usually pose different requirements for electron probe properties. Due to the complex, nonlinear and correlated nature of accelerator systems, electron beam property optimization is a time-taking process and often relies on extensive hand-tuning by experienced human operators. Algorithm based efficient online tuning strategies are highly desired. Here, we demonstrate multi-objective Bayesian active learning for speeding up online beam tuning at the SLAC MeV-UED facility. The multi-objective Bayesian optimization algorithm was used for efficiently searching the parameter space and mapping out the Pareto Fronts which give the trade-offs between key beam properties. Such scheme enables an unprecedented overview of the global behavior of the experimental system and takes a significantly smaller number of measurements compared with traditional methods such as a grid scan. This methodology can be applied in other experimental scenarios that require simultaneously optimizing multiple objectives by explorations in high dimensional, nonlinear and correlated systems.

43 PARTICLE ACCELERATORS↗
DOE OSTI2022

Coupled Electronic and Nuclear Motions during Azobenzene Photoisomerization Monitored by Ultrafast Electron Diffraction

Ultrafast electron diffraction is a powerful technique that can resolve molecular structures with femtosecond and angstrom resolutions. We demonstrate theoretically how it can be used to monitor conical intersection dynamics in molecules. Specific contributions to the signal are identified which vanish in the absence of vibronic coherence and offer a direct window into conical intersection paths. A special focus is on hybrid scattering from nuclei and electrons, a process that is unique to electron (rather than X-ray) diffraction and monitors the strongly coupled nuclear and electronic motions in the vicinity of conical intersections. Furthermore, an application is made to the cis to trans isomerization of azobenzene, computed with exact quantum dynamics wavepacket propagation in a reactive two-dimensional nuclear space.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Unsupervised anomaly detection in MeV ultrafast electron diffraction

MeV ultrafast electron diffraction (MUED) is a pump-probe technique used to study the dynamic structural evolution of materials. An ultrashort laser pulse triggers structural changes, which are then probed by an ultrashort relativistic electron beam. To overcome low signal-to-noise ratios, diffraction patterns are averaged over thousands of shots. However, shot-to-shot instabilities in the electron beam can distort individual patterns, introducing uncertainty. Improving MUED accuracy requires detecting and removing these anomalous patterns from large datasets. In this work, we developed a fully unsupervised methodology for the detection of anomalous diffraction patterns. Using a convolutional autoencoder, we calculate the reconstruction mean squared error of the diffraction patterns. Based on the statistical analysis of this error, we provide the user an estimation of the probability that the pattern is normal, which also allows a posterior visual inspection of the images that are difficult to classify. This method has been trained with only 100 diffraction patterns and tested on 1521 patterns, resulting in a false positive rate between 0.2% and 0.4%, with a training time of 10 s per image and a test time of about 1 s per image. Here, the proposed methodology can also be applied to other diffraction techniques in which large datasets are collected that include faulty images due to instrumental instabilities.

43 PARTICLE ACCELERATORS↗
DOE OSTI2016

Single-shot mega-electronvolt ultrafast electron diffraction for structure dynamic studies of warm dense matter

We have developed a single-shot mega-electronvolt ultrafast-electron-diffraction system to measure the structural dynamics of warm dense matter. The electron probe in this system is featured by a kinetic energy of 3.2 MeV and a total charge of 20 fC, with the FWHM pulse duration and spot size at sample of 350 fs and 120 μm respectively. We demonstrate its unique capability by visualizing the atomic structural changes of warm dense gold formed from a laser-excited 35-nm freestanding single-crystal gold foil. The temporal evolution of the Bragg peak intensity and of the liquid signal during solid-liquid phase transition are quantitatively determined. This experimental capability opens up an exciting opportunity to unravel the atomic dynamics of structural phase transitions in warm dense matter regime.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2019

The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction

The ultrafast photoinduced ring-opening of 1,3-cyclohexadiene constitutes a textbook example of electrocyclic reactions in organic chemistry and a model for photobiological reactions in vitamin D synthesis. Although the relaxation from the photoexcited electronic state during the ring-opening has been investigated in numerous studies, the accompanying changes in atomic distance have not been resolved. With this work, we present a direct and unambiguous observation of the ring-opening reaction path on the femtosecond timescale and subångström length scale using megaelectronvolt ultrafast electron diffraction. We followed the carbon–carbon bond dissociation and the structural opening of the 1,3-cyclohexadiene ring by the direct measurement of time-dependent changes in the distribution of interatomic distances. We discovered a substantial acceleration of the ring-opening motion after internal conversion to the ground state due to a steepening of the electronic potential gradient towards the product minima. The ring-opening motion transforms into rotation of the terminal ethylene groups in the photoproduct 1,3,5-hexatriene on the subpicosecond timescale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

A novel nondestructive diagnostic method for mega-electron-volt ultrafast electron diffraction

Abstract A real-time, nondestructive, Bragg-diffracted electron beam energy, energy-spread and spatial-pointing jitter monitor is experimentally verified by encoding the electron beam energy and spatial-pointing jitter information into the mega-electron-volt ultrafast electron diffraction pattern. The shot-to-shot fluctuation of the diffraction pattern is then decomposed to two basic modes, i.e., the distance between the Bragg peaks as well as its variation (radial mode) and the overall lateral shift of the whole pattern (drift mode). Since these two modes are completely decoupled, the Bragg-diffraction method can simultaneously measure the shot-to-shot energy fluctuation from the radial mode with 2·10 −4 precision and spatial-pointing jitter from the drift mode having wide measurement span covering energy jitter range from 10 −4 to 10 −1 . The key advantage of this method is that it allows us to extract the electron beam energy spread concurrently with the ongoing experiment and enables online optimization of the electron beam especially for future high charge single-shot ultrafast electron diffraction (UED) and ultrafast electron microscopy (UEM) experiments. Furthermore, real-time energy measurement enables the filtering process to remove off-energy shots, improving the resolution of time-resolved UED. As a result, this method can be applied to the entire UED user community, beyond the traditional electron beam diagnostics of accelerators used by accelerator physicists.

43 PARTICLE ACCELERATORS↗
DOE OSTI2018

Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction

The ultrafast laser excitation of matters leads to nonequilibrium states with complex solid-liquid phase-transition dynamics. In this paper, we used electron diffraction at mega–electron volt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 to 1000 picoseconds, transitioning to homogeneous melting that occurs catastrophically within 10 to 20 picoseconds at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Finally, our results constrain the electron-ion coupling rate, determine the Debye temperature, and reveal the melting sensitivity to nucleation seeds.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Vector-based feedback of continuous wave radiofrequency compression cavity for ultrafast electron diffraction

The temporal resolution of ultrafast electron diffraction at weakly relativistic beam energies (⁠≲100 keV) suffers from space-charge induced electron pulse broadening. We describe the implementation of a radio frequency (RF) cavity operating in the continuous wave regime to compress high repetition rate electron bunches from a 40.4 kV DC photoinjector for ultrafast electron diffraction applications. Active stabilization of the RF amplitude and phase through a feedback loop based on the demodulated in-phase and quadrature components of the RF signal is demonstrated. This scheme yields 144 ± 19 fs RMS temporal resolution in pump–probe studies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Femtosecond gas-phase mega-electron-volt ultrafast electron diffraction

The development of ultrafast gas electron diffraction with nonrelativistic electrons has enabled the determination of molecular structures with atomic spatial resolution. It has, however, been challenging to break the picosecond temporal resolution barrier and achieve the goal that has long been envisioned—making space- and-time resolved molecular movies of chemical reaction in the gas-phase. Recently, an ultrafast electron diffraction (UED) apparatus using mega-electron-volt (MeV) electrons was developed at the SLAC National Accelerator Laboratory for imaging ultrafast structural dynamics of molecules in the gas phase. The SLAC gas-phase MeV UED has achieved 65 fs root mean square temporal resolution, 0.63 Å spatial resolution, and 0.22 Å−1 reciprocal-space resolution. Such high spatial-temporal resolution has enabled the capturing of real-time molecular movies of fundamental photochemical mechanisms, such as chemical bond breaking, ring opening, and a nuclear wave packet crossing a conical intersection. In this paper, the design that enables the high spatial-temporal resolution of the SLAC gas phase MeV UED is presented. The compact design of the differential pump section of the SLAC gas phase MeV UED realized five orders-of-magnitude vacuum isolation between the electron source and gas sample chamber. The spatial resolution, temporal resolution, and long-term stability of the apparatus are systematically characterized.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction

The ultrafast laser excitation of matters leads to non-equilibrium states with complex solid-liquid phase transition dynamics. We used electron diffraction at mega-electronvolt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 ps to 1000 ps, transitioning to homogeneous melting that occurs catastrophically within 10-20 ps at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Our results constrain the electron-ion coupling rate, determine the Debye temperature and reveal the melting sensitivity to nucleation seeds.

Source record↗
DOE OSTI2022

Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations

In ultrafast electron diffraction (UED) experiments, accurate retrieval of time-resolved structural parameters, such as atomic coordinates and thermal displacement parameters, requires an accurate scattering model. Unfortunately, kinematical models are often inaccurate even for relativistic electron probes, especially for dense, oriented single crystals where strong channeling and multiple scattering effects are present. This article introduces and demonstrates dynamical scattering models tailored for quantitative analysis of UED experiments performed on single-crystal films. As a case study, we examine ultrafast laser heating of single-crystal gold films. Comparison of kinematical and dynamical models reveals the strong effects of dynamical scattering within nm-scale films and their dependence on sample topography and probe kinetic energy. Applying to UED experiments on an 11 nm thick film using 750 keV electron probe pulses, the dynamical models provide a tenfold improvement over a comparable kinematical model in matching the measured UED patterns. Also, the retrieved lattice temperature rise is in very good agreement with predictions based on previously measured optical constants of gold, whereas fitting the Debye–Waller factor retrieves values that are more than three times lower. Altogether, these results show the importance of a dynamical scattering theory for quantitative analysis of UED and demonstrate models that can be practically applied to single-crystal materials and heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Imaging the photochemistry of cyclobutanone using ultrafast electron diffraction: Experimental results

We investigated the ultrafast structural dynamics of cyclobutanone following photoexcitation at λ = 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 ± 0.2) ps toward 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 ± 0.05) ps with respect to 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 ± 0.2) ps via two rival fragmentation channels yielding ketene and ethylene, or propene and carbon monoxide. Furthermore, our study showcases the value of both 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 with such simulations.

Carbon monoxide↗
DOE OSTI2023

Design and construction of a compact, high-repetition-rate ultrafast electron diffraction instrument

We present the design and performance of a compact ultrafast electron diffraction instrument. The diffractometer provides a means of examining time-resolved ultrafast dynamical properties of solids. The system’s utilization is discussed in terms of instrument parameters and diffraction data from selected condensed matter samples. Here, the difractometer’s performance is highlighted in terms of detection sensitivity, instrumental temporal resolution, and the electron beam transverse coherence length. Following specific details of the construction, we present a practical discussion of parameters such as repetition rate and provide advice on general construction approaches for laboratory-based, keV ultrafast electron diffractometers. In addition, design guidance for constructing a compact electron gun source that is well-suited for studying diffraction from hard condensed matter is given. A unique data acquisition scheme, utilizing high laser repetition rates, is presented.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Calculation of rf-induced temporal jitter in ultrafast electron diffraction

A significant contribution to the temporal resolution of an ultrafast electron diffraction (UED) instrument is arrival time jitter caused by amplitude and phase variation of radio-frequency (rf) cavities. In this paper, we present a semianalytical approach for calculating rf-induced temporal jitter from klystron and rf cavity parameters. Our approach allows fast estimation of temporal jitter for MeV-UED beamlines and can serve as a virtual timing tool when shot-to-shot measurements of rf amplitude and phase jitters are available. A simulation study for the SLAC MeV-UED instrument is presented, and the temporal resolution of several beamline configurations is compared.

47 OTHER INSTRUMENTATION↗