Dynamically preferred state with strong electronic fluctuations from electrochemical synthesis of sodium manganate
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99 GENERAL AND MISCELLANEOUS↗
SEARCH · Engineering Papers
Results for “electron dynamics”
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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Dynamic Aperture of the EIC Electron Storage Ring
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Nosochkov, Y. M.↗
Lumped Parameter Modeling for Rapid Vibration Response Prototyping and Test Correlation for Electronic Units
Present preliminary work using lumped parameter models to approximate dynamic response of electronic units to random vibration; Derive a general N-DOF model for application to electronic units; Illustrate parametric influence of model parameters; Implication of coupled dynamics for unit/board design; Demonstrate use of model to infer printed wiring board (PWB) dynamics from external chassis test measurement.
random vibration↗
Role of matrix elements in the time-resolved photoemission signal
Time- and angle-resolved photoemission spectroscopy (TR-ARPES) provides access to the ultrafast evolution of electrons andmany-body interactions in solid-state systems. However, themomentum- and energy-resolved transient photoemission intensitymay not be unambiguously described by the intrinsic relaxation dynamics of photoexcited electrons alone.The interpretation of the time-dependent photoemission signal can be affected by the transient evolution of the electronic distribution, and both the one-electron removal spectral function aswell as the photoemissionmatrix elements. Here we investigate the topological insulator Bi 1.1 Sb 0.9 Te 2 S to demonstrate, bymeans of a detailed probe-polarization dependent study, the transient contribution ofmatrix elements toTR-ARPES.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Adaptive Ensemble Refinement of Protein Structures in High Resolution Electron Microscopy Density Maps with Radical Augmented Molecular Dynamics Flexible Fitting
Recent advances in cryo-electron microscopy (cryo-EM) have enabled modeling macromolecular complexes that are essential components of the cellular machinery. The density maps derived from cryo-EM experiments are often integrated with manual, knowledge or artificial intelligence driven, and physics-guided computational methods to build, fit, and refine molecular structures. Going beyond a single stationary- structure determination scheme, it is becoming more common to interpret the experimental data with an ensemble of models, which contributes to an average observation. Hence, there is a need to decide on the quality of an ensemble of protein structures on-the-fly, while refining them against the density maps. Here, we introduce such an adaptive decision making scheme during the molecular dynamics flexible fitting (MDFF) of biomolecules. Using RADICAL-Cybertools, and the new RADICAL augmented MDFF implementation (R-MDFF) is examined in high-performance computing environments for refinement of two protein systems, Adenylate Kinase and Carbon Monoxide Dehydrogenase. For the test cases, use of multiple replicas in flexible fitting with adaptive decision making in R-MDFF improves the overall correlation to the density by 40% relative to the refinements of the brute-force MDFF. The improvements are particularly significant at high, 2 - 3 Å, map resolutions. More importantly, the ensemble model captures key features of biologically relevant molecular dynamics that is inaccessible to a single-model interpretation. Finally, the pipeline is applicable to systems of growing sizes, which is demonstrated using ensemble refinement of capsid proteins from Chimpanzee adenovirus. The overhead for decision making remaining low and robust to computing environments. The software is publicly available on GitHub and includes a short user guide to install the R-MDFF on different computing environments, from local Linux based workstations to High Performance Computing (HPC) environments.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Manipulating and Probing Ultrafast Atomic and Molecular Dynamics (Final Report)
This program has focused on the exploration and control of dynamics in atoms, small molecules, clusters, and micro- or nano-structures following ultrafast excitation and/or driven by strong oscillating fields. In our principal experiments, gas phase atoms and molecules were exposed to short pulses of electromagnetic radiation with frequencies ranging from THz into the XUV spectral regions, and with durations from picoseconds to attoseconds. The pulses coherently induce and/or probe dynamics in the electronic, vibrational, and rotational degrees of freedom of the targets. The overarching goal of the various projects has been to exploit strong-field processes and/or implement novel ultrafast techniques for manipulating and probing coherent electronic and nuclear motion. Typically, the relevant system evolution occurs over attosecond to picosecond timescales. In doing so, we have gained a more complete picture of correlated multi-particle dynamics in atoms, molecules, and other complex systems and expanded the toolbox of useful techniques for manipulating and probing those dynamics. Grant funds were primarily used to: (i) pay salaries and fringe benefits for the PI and postdocs and stipends, tuition, and health care costs for graduate students; (ii) cover travel expenses for the PI, postdocs, and students to attend and participate in professional meetings, conferences, and workshops; and (iii) purchase research materials, supplies, and equipment required for experiments. The research resulted in the publication of 24 peer reviewed articles (including 1 in Nature Physics, 2 in Nature Communications, 7 in Physical Review Letters, and 12 in Physical Review A), and 4 PhD dissertations. The specific results from different funding periods are summarized separately in the main report.
74 ATOMIC AND MOLECULAR PHYSICS↗
Direct observation of chirality-induced spin selectivity in electron donor–acceptor molecules
The role of chirality in determining the spin dynamics of photoinduced electron transfer in donor-acceptor molecules remains an open question. Although chirality-induced spin selectivity (CISS) has been demonstrated in molecules bound to substrates, experimental information about whether this process influences spin dynamics in the molecules themselves is lacking. Here we used time-resolved electron paramagnetic resonance spectroscopy to show that CISS strongly influences the spin dynamics of isolated covalent donor–chiral bridge–acceptor (D-Bχ-A) molecules in which selective photoexcitation of D is followed by two rapid, sequential electron-transfer events to yield D •+ -Bχ-A •– . Exploiting this phenomenon affords the possibility of using chiral molecular building blocks to control electron spin states in quantum information applications.
Science & Technology - Other Topics↗
Properties of low-energy electron precipitation in the cleft during periods of unusually high ambient electron temperatures
A recently developed automated fitting procedure for Dynamics Explorer 2 electron energy spectra represents each auroral electron spectrum as a superposition of several Maxwellian and several Gaussian components. The fitting parameters give a digital representation which uniquely describes each spectrum. It is shown that unusually high ambient electron temperatures (of the order of 10,000 K) in the cleft are strongly correlated with the intensity parameters of the lowest-temperature Maxwellian components of the precipitation. The collisional heat input into the ambient electrons by these Maxwellian components of the precipitation fluxes is shown to be more than an order of magnitude higher in the high-temperature storm time cases than it is in a control set of 'normal temperature' quiet time cases. The heating effect of the solar flux is shown to be nearly the same for both sets of cases. As a result it is concluded that electron precipitation is the chief mechanism responsible for those high ambient temperatures.
Fontheim, Ernest G.↗
Imaging nanoscale carrier, thermal, and structural dynamics with time-resolved and ultrafast electron energy-loss spectroscopy
Time-resolved and ultrafast electron energy-loss spectroscopy (EELS) is an emerging technique for measuring photoexcited carriers, lattice dynamics, and near-fields across femtosecond to microsecond timescales. When performed in either a specialized scanning transmission electron microscope or ultrafast electron microscope (UEM), time-resolved and ultrafast EELS can directly image charge carriers, lattice vibrations, and heat dissipation following photoexcitation or applied bias. Yet, recent advances in theoretical calculations and electron optics are often required to realize the full potential of ultrafast EEL spectrum imaging. Here, in this review, we present a comprehensive overview of the recent progress in the theory and instrumentation of time-resolved and ultrafast EELS. We begin with an introduction to the technique, followed by a physical description of the loss function. We outline approaches for calculating and interpreting ground-state and transient EEL spectra spanning low-loss plasmons to core-level excitations analogous to x-ray absorption. We then survey the current state of time-resolved and ultrafast EELS techniques beyond photon-induced near-field electron microscopy, highlighting abilities to image carrier and thermal dynamics. Finally, we examine future directions enabled by emerging technologies, including electron beam monochromation, in situ and operando cells, laser-free UEM, and high-speed direct electron detectors. These advances position time-resolved and ultrafast EELS as a critical tool for uncovering nanoscale dynamic processes in quantum materials and solar energy conversion devices.
Computational methods↗
Simulation of decelerating streamers in inhomogeneous atmosphere with implications for runaway electron generation
The dynamics of positive and negative streamers is numerically simulated in atmospheric pressure air in the range of parameters corresponding to the streamer deceleration and termination in the middle of the discharge gap. A detailed comparison with experiments in air at constant and variable density demonstrates good agreement between the 2D simulation results and the observations. It is shown that positive and negative streamers behave in radically different ways when decelerating and stopping. When the head potential drops, the negative streamer transits to the mode in which the propagation is due to the forward electron drift. In this case, the radius of the ionization wave front increases, whereas the electric field at the streamer head decreases further and the streamer stops. Its head diameter continues to increase due to the slow drift of free electrons in the residual under-breakdown field. On the contrary, the only advancement mechanism for a positive streamer with a decreasing head potential is a decrease in the effective radius of the ionization wave, leading to a local increase in the electric field. This mechanism makes it possible to compensate for the reduction in the efficiency of gas photoionization at small head diameters. A qualitative 1D model is suggested to describe streamer deceleration and stopping for different discharge polarities. Estimates show that, during positive streamer stopping, the local electric field at the streamer head can exceed the threshold corresponding to the transition of electrons to the runaway mode when the head potential (relative to the surrounding space) decreases to~1.2 kV in atmospheric pressure air. In this case, pulsed generation of a beam of runaway electrons directed into the channel of a stopping positive streamer can occur. The energy of the formed pulsed electron beam depends on the intensity of photoionization in front of the streamer head. This energy can vary from 700 V (when increasing the photoionization rate by a factor of 10 with respect to the value in atmospheric pressure air) to 2.6 kV (when decreasing the photoionization rate by a factor of 1000). It is possible that this behavior of decelerating positive streamers can explain the observed bursts of x-ray radiation during the streamer propagation in long air gaps.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Electron Correlation and High-Temperature Superconductivity
Strong electron correlation plays a central role in the high-temperature superconductivity (HTSC) of cuprates. However, to date, research has focused only on its role in spin dynamics and related effects, even though it is becoming increasingly clear that spin alone may not be sufficient to create HTSC. Here, we discuss a possible role of electron correlation in the Bose–Einstein condensation (BEC) of Cooper pairs. Recently, we succeeded in observing dynamic electron correlation via inelastic X-ray scattering through results presented in real space. We discovered that electron correlations are strongly modified in the plasmon, proving that electron dynamics significantly affect electron correlation. Earlier, we found that in 4 He, the atom–atom distance in the BE condensate is 10% longer than that in the non-condensate. These results suggest the possibility that the reduction in electron-repulsion energy upon BEC is driving T c to high values. Thus, electron correlation itself could be the origin of the HTSC phenomenon.
Bose–Einstein condensation↗
Picosecond Carrier Dynamics in InAs and GaAs Revealed by Ultrafast Electron Microscopy
Understanding the limits of spatio-temporal carrier dynamics, especially in III-V semiconductors, is key to designing ultrafast and ultra-small optoelectronic components. However, identifying such limits and the properties controlling them has been elusive. Here, using scanning ultrafast electron microscopy (SUEM), in bulk n-GaAs and p-InAs, we simultaneously measure picosecond carrier dynamics along with three related quantities: sub-surface band bending, above-surface vacuum potentials, and surface trap densities. We make two surprising observations. First, we uncover a negative-time contrast in secondary electrons resulting from an interplay among these quantities. Second, despite dopant concentrations and surface state densities differing by many orders of magnitude between the two materials, their carrier dynamics, measured by photo-excited band bending and filling of surface states, occur at a seemingly common timescale of about 100 ps. This observation may indicate fundamental kinetic limits tied to a multitude of material and surface properties of optoelectronic III-V semiconductors, and highlights the need for techniques that simultaneously measure electro-optical kinetic properties.
36 MATERIALS SCIENCE↗
Tracking the ultraviolet-induced photochemistry of thiophenone during and after ultrafast ring opening
Photoinduced isomerization reactions lie at the heart of many chemical processes in nature. The mechanisms of such reactions are determined by a delicate interplay of coupled electronic and nuclear dynamics occurring on the femtosecond scale, followed by the slower redistribution of energy into different vibrational degrees of freedom. In this study, we apply time-resolved photoelectron spectroscopy with a seeded extreme ultraviolet free-electron laser to trace the ultrafast ring opening of gas-phase thiophenone molecules following ultraviolet photoexcitation. When combined with ab initio electronic structure and molecular dynamics calculations of the excited- and ground-state molecules, the results provide insights into both the electronic and nuclear dynamics of this fundamental class of reactions. The initial ring opening and non-adiabatic coupling to the electronic ground state are shown to be driven by ballistic S–C bond extension and to be complete within 350 fs. Theory and experiment also enable visualization of the rich ground-state dynamics that involve the formation of, and interconversion between, ring-opened isomers and the cyclic structure, as well as fragmentation over much longer timescales.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN
First-principles calculations of $\textit{e}$-ph interactions are becoming a pillar of electronic structure theory. However, the current approach is incomplete. The piezoelectric (PE) $\textit{e}$-ph interaction, a long-range scattering mechanism due to acoustic phonons in noncentrosymmetric polar materials, is not accurately described at present. Current calculations include short-range $\textit{e}$-ph interactions (obtained by interpolation) and the dipolelike Frölich long-range coupling in polar materials, but lack important quadrupole effects for acoustic modes and PE materials. Here we derive and compute the long-range $\textit{e}$-ph interaction due to dynamical quadrupoles, and apply this framework to investigate $\textit{e}$-ph interactions and the carrier mobility in the PE material wurtzite GaN. In this work, we show that the quadrupole contribution is essential to obtain accurate $\textit{e}$-ph matrix elements for acoustic modes and to compute PE scattering. Our work resolves the outstanding problem of correctly computing $\textit{e}$-ph interactions for acoustic modes from first principles, and enables studies of $\textit{e}$-ph coupling and charge transport in PE materials.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Excited-state dynamics of CH 2 I 2 and CH 2 IBr studied with UV-pump VUV-probe momentum-resolved photoion spectroscopy
We perform time-resolved ionization spectroscopy measurements of the excited state dynamics of CH 2 I 2 and CH 2 IBr following photoexcitation in the deep UV. The fragment ions produced by ionization with a vacuum-ultraviolet probe pulse are measured with velocity map imaging, and the momentum resolved yields are compared with trajectory surface hopping calculations of the measurement observable. Together with recent time-resolved photoelectron spectroscopy measurements of the same dynamics, these results provide a detailed picture of the coupled electronic and nuclear dynamics involved. Overall, our measurements highlight the non-adiabatic coupling between electronic states, which leads to notable differences in the dissociation dynamics for the two molecules.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A new paradigm in electron microscopy: Automated microstructure analysis utilizing a dynamic segmentation convolutional neutral network
Over the past half century, the transmission electron microscope enabled insight into the fundamental arrangements and structures of materials. State-of-the-art electron microscopes can acquire large image datasets across multiple imaging modalities. However, the manual annotation process for feature or defect quantification may not be feasible with the modern microscope. Convolutional neural networks emerged to characterize individual microstructural features from an image in a cost-effective, consistent manner. However, many of these neural network approaches rely on thousands to hundreds of thousands of manual annotations of each feature type across hundreds of images to train the network for adequate performance. This work focused on the development and application of a pixel-wise defect detection machine-learning dynamic segmentation convolutional neural network with associated automated acquisition and postprocessing to identify microstructural features rapidly and quantitatively from a small initial dataset incorporating multiple imaging modes. The approach was demonstrated for characterization of superalloy 718 from both single image acquisition on multiple detectors to in-situ evolution captured with a single detector on a standard desktop computer to demonstrate the low barrier to entry required for widespread adoption. Pixel-by-pixel class identification was excellent with strong identification of chemically distinct phases, structurally distinct phases, and defect structures, thus demonstrating the new paradigm of machine learning-assisted characterization.
36 MATERIALS SCIENCE↗
Bridging length scales in organic mixed ionic–electronic conductors through internal strain and mesoscale dynamics
Understanding the structural and dynamic properties of disordered systems at the mesoscale is crucial. This is particularly important in organic mixed ionic-electronic conductors (OMIECs), which undergo significant and complex structural changes when operated in an electrolyte. Here, in this study, we investigate the mesoscale strain, reversibility and dynamics of a model OMIEC material under external electrochemical potential using operando X-ray photon correlation spectroscopy. Our results reveal that strain and structural hysteresis depend on the sample's cycling history, establishing a comprehensive kinetic sequence bridging the macroscopic and microscopic behaviours of OMIECs. Furthermore, we uncover the equilibrium and non-equilibrium dynamics of charge carriers and material-doping states, highlighting the unexpected coupling between charge carrier dynamics and mesoscale order. These findings advance our understanding of the structure-dynamics-function relationships in OMIECs, opening pathways for designing and engineering materials with improved performance and functionality in non-equilibrium states during device operation. Understanding mesoscale structure and dynamics in organic mixed ionic-electronic conductors is crucial. Mesoscale strain kinetics and structural hysteresis have been studied, and they uncover the coupling between charge carrier dynamics and mesoscale order in organic mixed ionic-electronic conductors.
36 MATERIALS SCIENCE↗
Adiabatic behavior of an elliptical vortex in a time-dependent external strain flow
The adiabatic behavior of two-dimensional (2D) fluid vortices subject to slowly varying, time-dependent external strain flows is studied theoretically, and experimentally using magnetized non-neutral electron plasmas. Here the E × B drift dynamics of the electrons perpendicular to the magnetic field are analogous to the motion of fluid vorticity under the 2D Euler equations describing ideal fluids. A low-dimensional elliptical vortex patch model is used along with a WKB approximation to derive a formula for the breaking of an adiabatic invariant due to the changing external flow. The invariant is interpreted as the amplitude of a perturbative oscillation about a stable fixed point corresponding to a steady elliptical vortex. Smooth, hyperbolic tangent and piecewise linear ramp functions are considered for the external strain time dependence. Standard exponential breaking is observed in the former case, whereas the latter exhibits a power-law breaking curve with periodic modulation. It is found that a driving term in the equations of motion contributes the majority of the breaking whereas the frequency variation plays a weaker, but significant role. The experimental data agree closely with the theoretical model. The most significant deviation is due to inviscid damping behavior associated with the smooth edges of the experimental vortices, which tends to reduce the amplitude of the oscillation. Finally, the results are compared and contrasted with other related experimental, numerical, and theoretical work.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗