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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 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

The role of resonant nuclear modes in vibrationally assisted energy transport: The LHCII complex

In this paper, we discuss the explicit role of resonant nuclear/vibrational modes in mediating energy transport among chlorophylls in the Light-harvesting Complex II (LHCII), the major light-harvesting complex in green plants. The vibrational modes are considered to be resonant/quasi-resonant with the energy gap between electronic excitons. These resonant vibrations, along with the remaining nuclear degrees of freedom, constitute the environment/bath to the electronically excited system and contribute to two major phenomena: (a) decoherence and (b) incoherent phonon-mediated population relaxation. In this work, we explore the subtle interplay among the electronic excitation, the resonant vibrations, and the environment in dictating environment assisted quantum transport in light-harvesting complexes. We conclusively show that resonant vibrations are capable of boosting the incoherent population relaxation pathways and cause rapid decoherence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Defects in epitaxial Ru(0001) on Al2O3(0001): Dislocations, stacking faults, and deformation twins

In this study, defects in epitaxial Ru(0001) films on c-plane sapphire, with nominal thicknesses of 10–80 nm, deposited at 350 °C and step-annealed to 950 °C, were characterized using transmission electron microscopy. The variation of Ru and sapphire lattice parameters with temperature is such that the misfit strain for the observed 30° rotated-honeycomb epitaxial relationship is essentially constant with temperature at 1.5%, resulting in a biaxial stress of 10.0 GPa and an energy density of 150 MJ m –3 in unrelaxed films. Stress relaxation occurs by the formation of defects. For the 20–80 nm thick films, the defects are a- and c-type dislocations and stacking faults, argued to be of I 2 type. In addition, the films show the surprising presence of $\{11\bar{2}1\}1/3\langle11\bar{2}\bar{6}\rangle$ deformation twins. The 10 nm-thick films were found to be defect free. The critical thickness for misfit strain relaxation via the formation of threading and misfit dislocations is computed as 7±2 nm, depending on the choice of the dislocation core radius. Energetic analysis of twin formation, using both the infinite-matrix and the finite-matrix (Mori–Tanaka) approaches, provides values of the twin aspect ratios, assumed to be ellipsoidal, and shows that the latter but not the former approach can qualitatively explain the formation of the observed twins. In addition to providing the maximum strain relief compared to other potential twin types, $\{11\bar{2}1\}1/3\langle11\bar{2}\bar{6}\rangle$ twins do not require lattice shuffles and have a boundary that is a special boundary, namely, a 35° tilt boundary with a-type dislocations every other {0002} plane, that may also favor their formation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Tuning the dynamics in Fe 3 O 4 nanoparticles for hyperthermia optimization

The AC magnetic susceptibility (ACS) of Fe 3 O 4 nanoparticles was measured between 10 kHz and 4 MHz at different temperatures and in applied DC fields. In this frequency range, magnetostatic interactions impact magnetization dynamics even for dilute assemblies. The ACS spectrum of relaxation frequencies changes both with temperature and the addition of a small DC field. Because both the relaxation peak frequency and amplitude can be tuned with the DC field, these results could be applied to magnetic hyperthermia applications to optimize heat delivery.

Physics↗
DOE OSTI2020

A variational Monte Carlo approach for core excitations

In this work, we present a systematically improvable approach to core excitations in variational Monte Carlo. Building on recent work in excited-state-specific Monte Carlo, we show how a straightforward protocol, starting from a quantum chemistry guess, is able to capture core state's strong orbital relaxations, maintain accuracy in the near-nuclear region during these relaxations, and explicitly balance accuracy between ground and core excited states. In water, ammonia, and methane, which serve as prototypical representatives for oxygen, nitrogen, and carbon core states, respectively, this approach predicts core excitation energies within 0.3 eV of experiment and core excitation peak separations within 0.1 eV of experiment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Tuning the dynamics of imidazolium-based ionic liquids via hydrogen bonding. I. The viscous regime

Combining results from impedance spectroscopy and oscillatory shear rheology, this study focuses on the relation between the mass and charge flows and on how these are affected by the H-bonding in viscous ionic liquids (ILs). In particular, we compare the relaxational behaviors of the paradigmatic IL 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIM-TFSI) and its OH-functionalized counterpart 1-(2-hydroxyethyl)-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (OHEMIM-TFSI). Our results and their analysis demonstrate that the presence of cationic OH-groups bears a strong impact on the overall dynamics of OHEMIM-TFSI, although no signatures of suprastructural relaxation modes could be identified in their dielectric and mechanical responses. To check whether at the origin of this strong variation is the H-bonding or merely the difference between the corresponding cation sizes (controlling both the hydrodynamic volume and the inter-charge distance), the present study includes 1-propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (PMIM-TFSI), mixtures of EMIM-TFSI and PMIM-TFSI with lithium bis(trifluoromethylsulfonyl)imide (Li-TFSI), and mixtures of OHEMIM-TFSI with PMIM-TFSI. Their investigation clearly reveals that the dynamical changes induced by H-bonding are significantly larger than those that can be attributed to the change in the ion size. Moreover, in the mixtures of OHEMIM-TFSI with PMIM-TFSI, a dilution of the OH-groups leads to strong deviations from ideal mixing behavior, thus highlighting the common phenomenological ground of hydroxy-functionalized ILs and other H-bonded liquids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Further modeling of q 95 windows for the suppression of edge localized modes by resonant magnetic perturbations in the DIII-D tokamak

An improved resonant plasma response model that more accurately captures the physics of the interaction between a tokamak plasma and a resonant magnetic perturbation (RMP) is developed. The model interpolates between the linear and the nonlinear response regimes and takes into account the fact that the slip-frequency is non-zero in the nonlinear regime. The improved model is incorporated into the extended perturbed equilibrium code (EPEC) toroidal asymptotic matching code. The modified EPEC code is used to investigate RMP-induced edge-localized-mode (ELM) suppression in DIII-D H-mode discharge #145380. Somewhat surprisingly, allowing for a finite slip-frequency (i.e., relaxing the so-called no-slip constraint) is found to only slightly facilitate the locking of driven magnetic island chains to the RMP, and, hence, to only slightly facilitate RMP-induced ELM suppression. This is true despite the fact that the nature of non-locked island solutions is radically different when the no-slip constraint is imposed compared to when it is relaxed (in the first case, the widths of the island chains driven at the rational surfaces pulsate, and in the second case, they remain steady). The previously obtained conclusion that the response of a typical H-mode tokamak plasma to an RMP cannot be accurately modeled by linear theory is confirmed. Here, the previously obtained conclusion that the best agreement between theory and observations is achieved by assuming that the natural frequencies of tearing modes, in the absence of the RMP, are determined by the local equilibrium E × B velocity is also confirmed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Cavity molecular dynamics simulations of vibrational polariton-enhanced molecular nonlinear absorption

We report recent experiments have observed that the chemical and photophysical properties of molecules can be modified inside an optical Fabry– Pérot microcavity under collective vibrational strong coupling (VSC) conditions, and such modification is currently not well understood by theory. In an effort to understand the origin of such cavity-induced phenomena, some recent studies have focused on the effect of the cavity environment on the nonlinear optical response of the molecular subsystem. Here, we use a recently proposed protocol for classical cavity molecular dynamics simulations to numerically investigate the linear and the nonlinear response of liquid carbon dioxide under such VSC conditions following an optical pulse excitation. We find that applying a strong pulse of excitation to the lower hybrid light–matter state, i.e., the lower polariton (LP), can lead to an overall molecular nonlinear absorption that is enhanced by up to two orders of magnitude relative to the excitation outside the cavity. This polariton-enhanced multiphoton absorption also causes an ultrashort LP lifetime (0.2 ps) under strong illumination. Unlike usual polariton relaxation processes—whereby polaritonic energy transfers directly to the manifold of singly excited vibrational dark states—under the present mechanism, the LP transfers energy directly to the manifold of higher vibrationally excited dark states; these highly excited dark states subsequently relax to the manifold of singly excited states with a lifetime of tens of ps. Because the present mechanism is generic in nature, we expect these numerical predictions to be experimentally observed in different molecular systems and in cavities with different volumes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Compositionally graded Ga 1-x In x P buffers grown by static and dynamic hydride vapor phase epitaxy at rates up to 1 μm/min

Here, we demonstrate Ga 1-x In x P compositionally graded buffers (CGBs) grown on GaAs with lattice constants between GaAs and InP by hydride vapor phase epitaxy (HVPE). Growth rates were up to ~1 μm/min and threading dislocation density (TDD) was as low as 1.0 x 10 6 cm -2 . We studied the effect of substrate offcut direction, growth rate, and strain grading rate on CGB defect structure. We compared the effect of a “dynamic grading” style, which creates compositional interfaces via mechanical transfer of a substrate between two growth chambers, vs. “static grading” where the CGB grows in a single chamber. Dynamic grading yielded smoother grades with higher relaxation, but TDD was not significantly different between the two styles. Substrate offcut direction was the most important factor for obtaining CGBs with low defect density. (001) substrates offcut towards (111)B yielded smoother CGBs with lower TDD compared to CGBs grown on substrates offcut towards (111)A. Transmission electron microscopy of static and dynamic CGBs grown on A and B-offcuts only found evidence of phase separation in a static A-offcut CGB, indicating that the B offcut limits phase separation, which in turn keeps TDD low. Reduced growth rate led to the appearance CuPt-type atomic ordering, which affected the distribution of dislocations on the active glide planes but did not alter TDD. Higher growth rates led to smoother CGBs and did not appreciably increase TDD as otherwise predicted by steady-state models of plastic relaxation. These results show HVPE’s promise for lattice-mismatched applications and low-c ost InP virtual substrates on GaAs

36 MATERIALS SCIENCE↗
DOE OSTI2021

Valence shell photoelectron angular distributions and vibrationally resolved spectra of imidazole: A combined experimental–theoretical study

Linearly polarized synchrotron radiation has been used to record polarization dependent valence shell photoelectron spectra of imidazole in the photon energy range 21–100 eV. These have allowed the photoelectron angular distributions, as characterized by the anisotropy parameter β, and the electronic state intensity branching ratios to be determined. Complementing these experimental data, theoretical photoionization partial cross sections and β-parameters have been calculated for the outer valence shell orbitals. The assignment of the structure appearing in the experimental photoelectron spectra has been guided by vertical ionization energies and spectral intensities calculated by various theoretical methods that incorporate electron correlation and orbital relaxation. Strong orbital relaxation effects have been found for the 15a', nitrogen lone-pair orbital. The calculations also predict that configuration mixing leads to the formation of several low-lying satellite states. The vibrational structure associated with ionization out of a particular orbital has been simulated within the Franck–Condon model using harmonic vibrational modes. The adiabatic approximation appears to be valid for the X 2A" state, with the β-parameter for this state being independent of the level of vibrational excitation. However, for all the other outer valence ionic states, a disparity occurs between the observed and the simulated vibrational structure, and the measured β-parameters are at variance with the behavior expected at the level of the Franck–Condon approximation. Furthermore, these inconsistencies suggest that the excited electronic states may be interacting vibronically such that the nuclear dynamics occur over coupled potential energy surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Monte Carlo modeling of spin-polarized photoemission from p -doped bulk GaAs

Here, the anticorrelation between quantum efficiency (QE) and electron spin polarization (ESP) from a ρ-doped GaAs activated to negative electron affinity is studied in detail using an ensemble Monte Carlo approach. The photoabsorption, momentum and spin relaxation during transport, and tunneling of electrons through the surface potential barrier are modeled to identify fundamental mechanisms, which limit the efficiency of GaAs spin-polarized electron sources. In particular, we study the response of QE and ESP to various parameters, such as the photoexcitation energy, doping density, and electron affinity level. Our modeling results for various transport and emission characteristics are in good agreement with available experimental data. Our findings show that the behavior of both QE and ESP at room temperature can be fully explained by the bulk relaxation mechanisms and the time that electrons spend in the material before being emitted.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Dynamic strain evolution in an optically excited Pt thin film

The structural evolution of a Pt thin film following photo-thermal excitation by 1 ps optical laser pulses was studied with a time resolution of 100 ps over a total time period of 1 ms. Laser pulse fluences below 50 mJ/cm 2 were insufficient to relax the residual stress state of the as-prepared film even after 10 000 pulses. In this fluence regime, a rapid initial lattice expansion and a decrease in the lattice coherence length due to ultrafast photo-thermal heating were observed. The lattice expansion reached a maximum, and the coherence length reached a minimum, 100–200 ps after excitation before monotonically decaying back to their initial values in about 1 µs. Laser pulse fluences greater than 50 mJ/cm 2 produced irreversible stress relaxation within the first 10 optical pulses. In this regime, the lattice expansion was qualitatively similar to that in the low fluence regime, except that the initial structural state was not recovered. The evolution in the coherence length, however, was more complex. Following an initial decrease similar to that observed at low fluence, the coherence length then increased to a broad maximum greater than the initial value, before recovery.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Numerical study of $\delta$-function current sheets arising from resonant magnetic perturbations

We report general three-dimensional toroidal ideal magnetohydrodynamic equilibria with a continuum of nested flux surfaces are susceptible to forming singular current sheets when resonant perturbations are applied. The presence of singular current sheets indicates that, in the presence of non-zero resistivity, magnetic reconnection will ensue, leading to the formation of magnetic islands and potentially regions of stochastic field lines when islands overlap. Numerically resolving singular current sheets in the ideal magnetohydrodynamics (MHD) limit has been a significant challenge. This work presents numerical solutions of the Hahm–Kulsrud–Taylor (HKT) problem, which is a prototype for resonant singular current sheet formation. The HKT problem is solved by two codes: a Grad–Shafranov (GS) solver and the Stepped Pressure Equilibrium Code (SPEC) code. The GS solver has built-in nested flux surfaces with prescribed magnetic fluxes. The SPEC code implements multi-region relaxed magnetohydrodynamics (MRxMHD), whereby the solution relaxes to a Taylor state in each region while maintaining force balance across the interfaces between regions. As the number of regions increases, the MRxMHD solution appears to approach the ideal MHD solution assuming a continuum of nested flux surfaces. We demonstrate agreement between the numerical solutions obtained from the two codes through a convergence study.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Influence of strain and dislocations on GaSb/GaAs quantum dots: From nested to staggered band alignment

We investigate the influence of strain and dislocations on band alignment in GaSb/GaAs quantum dot systems. Composition profiles from cross-sectional scanning tunneling microscopy images are interpolated onto a finite element mesh in order to calculate the distribution of local elastic strain, which is converted to a spatially varying band alignment using deformation potential theory. Our calculations predict that dislocation-induced strain relaxation and charging lead to significant local variations in band alignment. Furthermore, misfit strain induces a transition from a nested (type I) to a staggered (type II) band alignment. Although dislocation-induced strain relaxation prevents the type I to type II transition, electrostatic charging at dislocations induces the staggered band alignment once again.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Partially polaron-transformed quantum master equation for exciton and charge transport dynamics

Polaron-transformed quantum master equation (PQME) offers a unified framework to describe the dynamics of quantum systems in both limits of weak and strong couplings to environmental degrees of freedom. Thus, the PQME serves as an efficient method to describe charge and exciton transfer/transport dynamics for a broad range of parameters in condensed or complex environments. However, in some cases, the polaron transformation (PT) being employed in the formulation invokes an over-relaxation of slow modes and results in premature suppression of important coherence terms. A formal framework to address this issue is developed in the present work by employing a partial PT that has smaller weights for low frequency bath modes. In this work, it is shown that a closed form expression of a second order time-local PQME including all the inhomogeneous terms can be derived for a general form of partial PT, although more complicated than that for the full PT. All the expressions needed for numerical calculation are derived in detail. Applications to a model of a two-level system coupled to a bath of harmonic oscillators, with test calculations focused on those due to homogeneous relaxation terms, demonstrate the feasibility and the utility of the present approach.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Laboratory study of the failed torus mechanism in arched, line-tied, magnetic flux ropes

Coronal mass ejections (CMEs) are some of the most energetic and violent events in our solar system. The prediction and understanding of CMEs are of particular importance due to the impact that they can have on Earth-based satellite systems and, in extreme cases, ground-based electronics. CMEs often occur when long-lived magnetic flux ropes (MFRs) anchored to the solar surface destabilize and erupt away from the Sun. One potential cause for these eruptions is an ideal magnetohydrodynamic (MHD) instability, such as the kink or torus instability. Previous experiments on the magnetic reconnection experiment revealed a class of MFRs that were torus-unstable but kink-stable, which failed to erupt. These “failed-tori” went through a process similar to Taylor relaxation, where the toroidal current was redistributed before the eruption ultimately failed. Herein we have investigated this behavior through additional diagnostics that measure the current distribution at the foot points and the energy distribution before and after an event. These measurements indicate that ideal MHD effects are sufficient to explain the energy distribution changes during failed torus events. This excludes Taylor relaxation as a possible mechanism of current redistribution during an event. A new model that only requires non-ideal effects in a thin layer above the electrodes is presented to explain the observed phenomena. This work broadens our understanding of the stability of MFRs and the mechanism behind the failed torus through the improved prediction of the torus instability and through new diagnostics to measure the energy inventory and current profile at the foot points.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Evolution of the age-included nearest pair distribution in disperse multiphase flows

The age of the nearest particle pair is introduced as the difference between the current time and the most recent time when the nearest particle pair was formed. The evolution equation for the age-included nearest pair distribution function is derived. With the assumption of random destruction of the nearest particle pairs, the evolution equation predicts the exponential probability distribution of the ages of the nearest particle pairs. Particle-resolved numerical simulations with moving particles are performed to verify this prediction. The equation is then used to derive the evolution equation for the particle–fluid–particle (PFP) stress, which is known to be related to hyperbolicity of the two-fluid equations. It is found that the relaxation time of the age probability distribution is also the relaxation time for the PFP stress. Guided by the closure terms in the PFP stress evolution equation, we study kinematics of the nearest particle pairs in the particle-resolved simulations for flows caused by sedimentation of the particles with initially isotropic and homogeneous particle distributions. At the steady states, the particle Reynolds numbers are around 20. Anisotropy and inhomogeneity of particle distributions are seen to develop in these flows. The mean distances to the nearest particles and evolution of the distribution of the Voronoi cell volumes are studied. We also found the PFP stress is closely related to the changes in these inter-particle scale quantities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Mechanistic origins of methyl-driven Overhauser DNP

The Overhauser effect in the dynamic nuclear polarization (DNP) of non-conducting solids has drawn much attention due to the potential for efficient high-field DNP as well as a general interest in the underlying principles that enable the Overhauser effect in small molecules. We recently reported the observation of 1 H and 2 H Overhauser effects in H 3 C- or D 3 C-functionalized Blatter radical analogs, which we presumed to be caused by methyl rotation. In this work, we look at the mechanism for methyl-driven Overhauser DNP in greater detail, considering methyl librations and tunneling in addition to classical rotation. Here, we predict the temperature dependence of these mechanisms using density functional theory and spin dynamics simulations. Comparisons with results from ultralow-temperature magic angle spinning-DNP experiments revealed that cross-relaxation at temperatures above 60 K originates from both libration and rotation, while librations dominate at lower temperatures. Due to the zero-point vibrational nature of these motions, they are not quenched by very low temperatures, and methyl-driven Overhauser DNP is expected to increase in efficiency down to 0 K, predominantly due to increases in nuclear relaxation times.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Optical-pump–terahertz-probe spectroscopy in high magnetic fields with kHz single-shot detection

We demonstrate optical pump–THz probe (OPTP) spectroscopy with a variable external magnetic field (0–9 T), in which the time-dependent THz signal is measured by echelon-based single-shot detection at a repetition rate of 1 kHz. The method reduces data acquisition times by more than an order of magnitude compared to conventional electro-optic sampling using a scanning delay stage. The approach illustrates the wide applicability of the single-shot measurement approach to non-equilibrium systems that are studied through OPTP spectroscopy, especially in cases where parameters such as magnetic field strength (B) or other experimental parameters are varied. We demonstrate the capabilities of our measurement by performing cyclotron resonance experiments in bulk silicon, where we observe B-field-dependent carrier relaxation and distinct relaxation rates for different carrier types. We use a pair of economical linear array detectors to measure 500 time points on each shot, offering an equivalent performance to camera-based detection with possibilities for higher repetition rates.

Instruments & Instrumentation↗