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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 271 records · Page 15

Shaping Micro-Bunched Electron Beams for Compact X-ray Free-Electron Lasers with Transverse Gradient Undulators

Laser-modulator-based micro-bunching of electron beams has been applied to many novel operating modes of X-ray free-electron lasers from harmonic generation to attosecond pulse production. Recently, it was also identified as a key enabling technology for the production of a compact XFEL driven by a relatively low-energy beam. In traditional laser modulator schemes with low-energy and high-current bunches, collective effects limit the possible working points that can be employed, and thus it is difficult to achieve optimal XFEL performance. We propose to utilize transverse longitudinal coupling in a transverse gradient undulator (TGU) to shape micro-bunched electron beams so as to optimize their performance in a compact X-ray free-electron laser. We show that a TGU added to a conventional laser modulator stage enables much more flexibility in the design, allowing one to generate longer micro-bunches less subject to slippage effects and even lower the slice emittance of the micro-bunches. We present a theoretical analysis of laser-based micro-bunching with an added TGU, simulation of compression with collective effects in such systems, and finally XFEL simulations demonstrating the gains in peak power enabled by the TGU. Although we focus on the application to compact XFELs, what we propose is a general phase space manipulation that may find utility in other applications as well.

eSASE↗

Electron Crescent Distributions as a Manifestation of Diamagnetic Drift in an Electron-Scale Current Sheet: Magnetospheric Multiscale Observations Using New 7.5 ms Fast Plasma Investigation Moments

We report Magnetospheric Multiscale observations of electron pressure gradient electric fields near a magnetic reconnection diffusion region using a new technique for extracting 7.5 ms electron moments from the Fast Plasma Investigation. We find that the deviation of the perpendicular electron bulk velocity from E × B drift in the interval where the out-of-plane current density is increasing can be explained by the diamagnetic drift. In the interval where the out-of-plane current is transitioning to in-plane current, the electron momentum equation is not satisfied at 7.5 ms resolution.

fast plasma↗

Probing Electron Beam Induced Transformations on a Single-Defect Level via Automated Scanning Transmission Electron Microscopy

A robust approach for real-time analysis of the scanning transmission electron microscopy (STEM) data streams, based on ensemble learning and iterative training (ELIT) of deep convolutional neural networks, is implemented on an operational microscope, enabling the exploration of the dynamics of specific atomic configurations under electron beam irradiation via an automated experiment in STEM. Combined with beam control, this approach allows studying beam effects on selected atomic groups and chemical bonds in a fully automated mode. Here, in this study, we demonstrate atomically precise engineering of single vacancy lines in transition metal dichalcogenides and the creation and identification of topological defects in graphene. The ELIT-based approach facilitates direct on-the-fly analysis of the STEM data and engenders real-time feedback schemes for probing electron beam chemistry, atomic manipulation, and atom by atom assembly.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photodissociation of aqueous I3− observed with liquid-phase ultrafast mega-electron-volt electron diffraction

Developing femtosecond resolution methods for directly observing structural dynamics is critical to understanding complex photochemical reaction mechanisms in solution. We have used two recent developments, ultrafast mega-electron-volt electron sources and vacuum compatible sub-micron thick liquid sheet jets, to enable liquid-phase ultrafast electron diffraction (LUED). We have demonstrated the viability of LUED by investigating the photodissociation of tri-iodide initiated with a 400 nm laser pulse. This has enabled the average speed of the bond expansion to be measured during the first 750 fs of dissociation and the geminate recombination to be directly captured on the picosecond time scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Complete collision data set for electrons scattering on molecular hydrogen and its isotopologues: III. Vibrational excitation via electronic excitation and radiative decay

We present state-resolved cross sections for vibrational excitation via electronic excitation followed by radiative decay (ERD), for electrons scattering on all bound vibrational levels of the ground electronic state ($X\hspace{1.5 mm} ^1Σ_g^+$) of molecular hydrogen and its isotopologues (H 2 , HD, HT, D 2 , DT and T 2 ). We consider excitation of the singlet $\textit{n}$ = 2–3 states (where n refers to the united-atoms-limit principle quantum number) and account for all possible decay pathways back to the bound vibrational levels of the ground electronic state ($X\hspace{1.5 mm} ^1Σ_g^+$) to produce an estimate for the ERD cross sections. A selection of the results are presented in graphical form and a full data set is provided as both numerical values and analytic fit functions in supplementary data files. The uncertainty in the cross sections is estimated to be 11%, except for scattering on the highest bound vibrational level of HD, HT, D 2 , and DT, where the uncertainty is 21%. The data can be downloaded from the MCCC database at mccc-db.org.

74 ATOMIC AND MOLECULAR PHYSICS↗

Multiparametric AFM Insights into Electron Transport Mechanisms in Biomemristors

Biomemristors have attracted significant attention due to their applications in biodegradable and flexible electronic devices, and their prospective functions in information storage, neural synapses, and neuromorphic computation. Hence, understanding biomaterials' resistive switching (RS) mechanism is essential to design novel biomemristors with enhanced performance. In the last decade, various atomic force microscopy (AFM) modes, such as Kelvin probe force microscopy (KPFM) and conductive atomic force microscopy (cAFM), in situ/operando visualize the electron transport behaviors within biomemristors at the nanoscale. This review provides a comprehensive discussion of multiparametric AFM techniques to characterize biomemristors and inspire new ideas in developing next-generation consumer electronics. We also summarize the progress of revealing the internal mechanism of biomemristors with functional AFM to visualize and understand the switching behavior. Finally, the opportunities and challenges of further utilizing multiparametric AFM to explore the electron transport mechanisms in biomemristors are presented.

Shi, Chenyang↗

Measurements of electron transport in liquid and gas Xenon using a laser-driven photocathode

Measurements of electron drift properties in liquid and gaseous xenon are reported. The electrons are generated by the photoelectric effect in a semitransparent gold photocathode driven in transmission mode with a pulsed ultraviolet laser. The charges drift and diffuse in a small chamber at various electric fields and a fixed drift distance of 2.0 cm. At an electric field of 0.5 kV/cm, the measured drift velocities and corresponding temperature coefficients respectively are 1.97 ± 0.04 mm/µs and (-0.69 ± 0.05)%/K for liquid xenon, and 1.42 ± 0.03 mm/µs and (+0.11 ± 0.01)%/K for gaseous xenon at 1.5 bar. In addition, we measure longitudinal diffusion coefficients of 25.7±4.6 cm2/s and 149±23 cm2/s, for liquid and gas, respectively. The quantum efficiency of the gold photocathode is studied at the photon energy of 4.73 eV in liquid and gaseous xenon, and vacuum. These charge transport properties and the behavior of photocathodes in a xenon environment are important in designing and calibrating future large scale noble liquid detectors.

Njoya, Oumarou↗

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↗

Electron Affinity and Electronic Structure of Hexafluoroacetone (HFA) Revealed by Photodetaching the [HFA] •– Radical Anion

A great deal of effort has been focused on developing a metal-free catalytic system for epoxidation of unreactive alkenes. Fluoroketones are thought as remarkably promising catalysts for epoxidation reactions. The combination of fluorinated alcohols and catalytic amounts of hexafluoroacetone (HFA) gives a versatile and effective medium for epoxidation of various olefins with hydrogen peroxide. However, the fundamental physicochemical properties of HFA remained largely unclear, although they were very important to understand the related interactions. Here, in this study, we performed a joint study on the electron affinity and electronic structure of HFA employing negative ion photoelectron (NIPE) spectroscopy and quantum chemistry calculations. Two distinct bands with complicated vibrational progressions were observed in the 193 nm NIPE spectrum. The adiabatic/vertical detachment energies (ADE/VDE) were derived to be 1.42/2.06 and 4.43/4.86 eV for the ground singlet state and excited triplet state, respectively. Using the optimized geometries and vibrational frequencies of the anion and the neutral, the Franck–Condon factors were calculated for electron detachments to produce HFA in its lowest singlet and triplet states. Good agreements are obtained hereby for both bands between the experimental and calculated NIPE spectra, when taking into account combination vibrational excitations, unequivocally revealing that HFA possesses a singlet ground state with a giant singlet–triplet energy difference (ΔE ST ). The electron affinity (EA) and ΔE ST of HFA were therefore determined to be EA = 1.42 ± 0.02 eV and ΔE ST = −3.01 eV.

Wang, Lei↗

The Low-Lying Electronic States of NO 2 : Potential Energy and Dipole Surfaces, Bound States, and Electronic Absorption Spectrum

Nitrogen dioxide, NO 2 , is a free radical composed of the two most abundant elements in Earth’s atmosphere, nitrogen and oxygen, and is relevant to atmospheric and combustion chemistry. The electronic structure of even its lowest-lying states is remarkably complex, with various conical intersections and Renner–Teller pairings, giving rise to complex and perturbed vibronic states. Here we report some analysis of the 18 molecular states of doublet spin-multiplicity formed by combining ground-state N( 4 S u ) and O( 3 P g ) atoms. In this work, three-dimensional potential energy surfaces were fit at the MRCI(Q)-F12/VTZ-F12 level, describing the lowest four ($\tilde X$, $\tilde A$, $\tilde B$, and $\tilde C$) electronic states. A properties-based diabatization procedure was applied to accommodate the intersections, producing energies in a quasidiabatic representation and yielding couplings that were also fit into surfaces. The low-lying vibrational levels on the ground $\tilde X$ state were computed and compared with experimental measurements. Compared to experiment, the lowest 125 calculated vibrational levels (up to 8500 cm –1 above the zero-point energy) have a root-mean-squared error of 16.5 cm –1 . In addition, dipole moments for each of the lowest four electronic states—and the transition dipoles between them—were also computed and fit. With the coupled energy and dipole surfaces, the electronic spectrum was calculated in absolute intensity and compared with experimental measurements. Detailed structure in the experimental spectrum was successfully reproduced, and the total integrated intensity matches experiment to an accuracy of ~1.5% with no empirical adjustments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Characteristics of Electron Precipitation During 40 Energetic Electron Injections Inferred via Subionospheric VLF Signal Propagation

Energetic electron injection events are associated with energetic electron precipitation (EEP) through possible resonant wave-particle interactions. Previous studies confirm the impacts of injection-driven precipitation on observed amplitude/phase of subionospheric VLF (very low frequency) signals transmitted from distant artificial transmitters. Currently, there are substantial uncertainties on precipitation characteristics and flux during injection events. In this work we study 40 injection events selected by Van Allen Probes particle data to investigate the changes in amplitude and phase of VLF signals at ground receivers across Canada during particle injection events. We model the ionospheric effect of the EEP flux to find its impact on VLF propagation and characterize the injection events. Typically, we find a clear phase advance of ~40° in the received VLF signal at Fort Smith (Canada, L = 8) transmitted from U.S. Navy communication transmitter NAA at Maine (USA). Comparing to other VLF transmitter-receiver paths in North America leads us to conclude that effects are only seen on paths with adequately large range >>200 km) through L > 7. Modeling the VLF phase change indicates that in the majority of events (>90%), less than 10% of the strong scattering limit inferred from particle flux measurements at the Van Allen Probes is required to obtain the observed VLF phase signature. The median precipitating flux during energetic particle injections is less than 4 × 10 6 el/cm 2 s sr (<10% of the strong scattering rate) for electrons above ~40 keV extracted from trapped particles energy spectrum. This implies that strong scattering is not typical for these 40 selected energetic electron injection events.

79 ASTRONOMY AND ASTROPHYSICS↗

Estimating Electron Temperature and Density Using Van Allen Probe Data: Typical Behavior of Energetic Electrons in the Inner Magnetosphere

Abstract The Earth's inner magnetosphere contains multiple electron populations influenced by different factors. The cold electrons of the plasmasphere, warm plasma that contributes to the ring current, and the relativistic plasma of the radiation belts often seem to behave independently. Using omni‐directional flux and energy measurements from the HOPE and Magnetic Electron Ion Spectrometer instruments aboard the Van Allen Probes, we provide a detailed density and temperature description of the inner magnetosphere, offering a comprehensive statistical analysis of the entire Van Allen Probe era. While number density and temperature data at geosynchronous orbit are available, this study focuses on the warm plasma in the inner magnetosphere . Values of density and temperature are extracted by fitting energy and phase space density to obtain the distribution function. The fitted distributions are related to the zeroth and second moments to estimate the number density and temperature. Analysis has indicated that a two Maxwellian fit is sufficient over a wide range of and that there are two independent plasma populations. The more energetic population has a median number density of approximately and a temperature of around 130 keV, with a temperature peak observed between L * = 4 and L * = 4.5. This population is relatively uniform in magnetic local time (MLT). In contrast, the less energetic warm electron population has a median number density of about and a temperature of 7.4 keV. Strong statistical trends in density and temperature across both L * and MLT are presented, along with potential sources driving these variations.

58 GEOSCIENCES↗

Manipulating electron redistribution to achieve electronic pyroelectricity in molecular [FeCo] crystals

Pyroelectricity plays a crucial role in modern sensors and energy conversion devices. However, obtaining materials with large and nearly constant pyroelectric coefficients over a wide temperature range for practical uses remains a formidable challenge. Attempting to discover a solution to this obstacle, we combined molecular design of labile electronic structure with the crystal engineering of the molecular orientation in lattice. This combination results in electronic pyroelectricity of purely molecular origin. Here, we report a polar crystal of an [FeCo] dinuclear complex exhibiting a peculiar pyroelectric behavior (a substantial sharp pyroelectric current peak and an unusual continuous pyroelectric current at higher temperatures) which is caused by a combination of Fe spin crossover (SCO) and electron transfer between the high-spin Fe ion and redox-active ligand, namely valence tautomerism (VT). As a result, temperature dependence of the pyroelectric behavior reported here is opposite from conventional ferroelectrics and originates from a transition between three distinct electronic structures. The obtained pyroelectric coefficient is comparable to that of polyvinylidene difluoride at room temperature.

36 MATERIALS SCIENCE↗

Liquid-phase mega-electron-volt ultrafast electron diffraction

The conversion of light into usable chemical and mechanical energy is pivotal to several biological and chemical processes, many of which occur in solution. To understand the structure–function relationships mediating these processes, a technique with high spatial and temporal resolutions is required. Here, we report on the design and commissioning of a liquid-phase mega-electron-volt (MeV) ultrafast electron diffraction instrument for the study of structural dynamics in solution. Limitations posed by the shallow penetration depth of electrons and the resulting information loss due to multiple scattering and the technical challenge of delivering liquids to vacuum were overcome through the use of MeV electrons and a gas-accelerated thin liquid sheet jet. To demonstrate the capabilities of this instrument, the structure of water and its network were resolved up to the 3rd hydration shell with a spatial resolution of 0.6 Å; preliminary time-resolved experiments demonstrated a temporal resolution of 200 fs.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Coherent high-power RF wakefield generation by electron bunch trains in a metamaterial structure

In this paper, we present an experimental study of coherent high-power wakefield generation in a metamaterial (MTM) structure at 11.7 GHz by 65 MeV electron bunch trains at the Argonne Wakefield Accelerator (AWA), following a previous experiment, the Stage-I experiment, at the AWA. Both the Stage-II experiment, reported in this paper, and the Stage-I experiment were conducted using MTM structures, which are all-metal periodic structures with the period being much smaller than the wavelength. Differences between the two experiments include (1) structure length (Stage-I 8 cm and Stage-II 20 cm); (2) number of bunches used to excite the structure (Stage-I with two bunches, up to 85 nC of total charge; Stage-II with eight bunches, up to 224 nC of total charge); and (3) highest peak power measured (Stage-I 80 MW in a 2 ns pulse and Stage-II 380 MW in a 10 ns pulse). High-power radio frequency pulses were generated by reversed Cherenkov radiation of the electron beam due to the negative group velocity in the MTM structures. Because the radiation is coherent, a train of bunches with a proper spacing can build up to achieve a high peak power. The observed output power levels are very promising for future applications in direct collinear wakefield acceleration or in transfer to a second accelerator for two-beam acceleration.

36 MATERIALS SCIENCE↗

Electronic heat generation in semiconductors: Non-equilibrium excitation and evolution of zone-edge phonons via electron–phonon scattering in photo-excited germanium

We investigate experimentally and using first-principles theory the generation of phonons and the relaxation of carriers on picosecond timescales across the Brillouin zone of photo-excited Ge by inter-valley electron–phonon scattering. The phonons generated are typical of those generated in semiconductor devices, contributing to the accumulation of heat within the material. We simulate the time-evolution of phonon populations, based on first-principles band structure and electron–phonon and phonon–phonon matrix elements, and compare them to data from time-resolved x-ray diffuse scattering experiments, performed at the Linac Coherent Light Source x-ray free-electron laser facility, following photo-excitation by a 50 fs near-infrared optical pulse. We show that the intensity of the non-thermal x-ray diffuse scattering signal, which is observed to grow substantially near the L-point of the Brillouin zone over 3–5 ps, is due to phonons generated by scattering of carriers between the Δ and L valleys. These phonons have low group velocities, resulting in a heat bottleneck. With the inclusion of phonon decay through 3-phonon processes, the simulations also account for other non-thermal features observed in the x-ray diffuse scattering intensity, which are due to anharmonic phonon–phonon scattering of the phonons initially generated by electron–phonon scattering.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Two-dimensional electronic–vibrational sum frequency spectroscopy for interactions of electronic and nuclear motions at interfaces

Significance Electronic–vibrational couplings are pivotal in many photo-induced processes at interfaces and surfaces. Two-dimensional electronic–vibrational sum frequency generation spectroscopy is a unique tool to decipher electronic–vibrational couplings for excited states of molecules at interfaces and surfaces, enabling the correlation of photo-induced electronic–vibrational manifolds with their subsequent time evolution of high-frequency vibrational modes. This technique is especially powerful to monitor ultrafast processes such as charge transfer, energy transfer, proton transfer, and proton-coupled charge transfer at interfaces and surfaces on a real-time basis.

Deng, Gang-Hua↗