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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 1,495 records · Page 83
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

The unusual symmetry of hexafluoro-o-xylene—A microwave spectroscopy and computational study

The rotational constants and quartic centrifugal distortion coefficients of hexafluoro-o-xylene were precisely derived from the 8 GHz to 18 GHz gas phase microwave spectrum. In addition, the rotational constants of all singly substituted 13 C isotopologues were determined. Instead of the intuitively expected symmetry of C 2v , as in o-xylene, calculations with a variety of methods (B3LYP, CAM-B3LYP, ωB97XD, MP2, and coupled-cluster singles, doubles, and perturbative triples) predict a C 2 symmetry structure in which the two CF 3 groups rotate in opposite directions by about 16°. While the experimental results in this study are not capable of proving this unusual symmetry, they can support future microwave, gas phase electron diffraction or nuclear magnetic resonance studies. From the presented data, a preliminary r 0 structure was determined, reproducing the experimental rotational constants with deviations of no more than 15 kHz. Analysis of the interactions between the two CF 3 groups using an effective fragment potential approach identifies two major contributions to their interaction, due to exchange-repulsion and electrostatic repulsion, with electrostatic repulsion responsible for the barrier at the C 2v geometry.

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

Atomistic study of silicon alloying in the spallation behavior of nanocrystalline aluminum systems

Here, the effect of concentration of the alloying element silicon (Si) on the shock and spall response of aluminum (Al) is studied using classical molecular dynamics (MD) simulations. Silicon is distributed as individual grains and as grain boundaries and the dynamic response under shock is studied for an impact velocity of 1000 m/s. A general trend observed here is that the spallation is almost exclusively intergranular and limited to Al-Si interfaces. The spall strengths are observed to a) decrease with an increase in alloying of Si as grains and b) show little increase for up to 50% grain boundary segregation. An increase in grain size of the whole system showed negligible differences in spall strength, highlighting the significance of concentration of the alloying species rather than its grain size. These results provide an atomistic understanding of light-weight metallic systems under shock compression and pave the way for designing multiphase metal matrix alloys and composites for defense/armor applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Watching a signaling protein function: What has been learned over four decades of time-resolved studies of photoactive yellow protein

Photoactive yellow protein (PYP) is a signaling protein whose internal p-coumaric acid chromophore undergoes reversible, light-induced trans-to-cis isomerization, which triggers a sequence of structural changes that ultimately lead to a signaling state. Since its discovery nearly 40 years ago, PYP has attracted much interest and has become one of the most extensively studied proteins found in nature. The method of time-resolved crystallography, pioneered by Keith Moffat, has successfully characterized intermediates in the PYP photocycle at near atomic resolution over 12 decades of time down to the sub-picosecond time scale, allowing one to stitch together a movie and literally watch a protein as it functions. But how close to reality is this movie? To address this question, results from numerous complementary time-resolved techniques including x-ray crystallography, x-ray scattering, and spectroscopy are discussed. Emerging from spectroscopic studies is a general consensus that three time constants are required to model the excited state relaxation, with a highly strained ground-state cis intermediate formed in less than 2.4 ps. Persistent strain drives the sequence of structural transitions that ultimately produce the signaling state. Crystal packing forces produce a restoring force that slows somewhat the rates of interconversion between the intermediates. Moreover, the solvent composition surrounding PYP can influence the number and structures of intermediates as well as the rates at which they interconvert. When chloride is present, the PYP photocycle in a crystal closely tracks that in solution, which suggests the epic movie of the PYP photocycle is indeed based in reality.

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

Experimental and modeling study of 1/ f noise in multilayer MoS2 and MoSe2 field-effect transistors

In field-effect transistors (FETs) with two-dimensional (2D) transition metal dichalcogenide channels, the dependence of field-effect mobility on atomic layer thickness has been studied and interpreted in terms of interface scattering and interlayer coupling resistance (Rint). However, a model for 1/f noise, such as in MoS2 and in MoSe2 FETs, for various contact metals and layer number thicknesses has not been reported. In this work, we have experimentally studied current–voltage and 1/f noise on MoS2 and MoSe2 FETs with source and drain contacts of high and low work function metals to understand both the mobility and the noise behavior. We have developed a noise model incorporating layer number dependent Hooge parameters and Rint. The noise and mobility models utilize screening lengths for charge, mobility, and Hooge parameter to describe the variation of these quantities with a layer number. Using our single model topology with appropriate fitting parameters for each material and each contact metal, the model captures the experimentally observed layer thickness dependence of the Hooge parameter. Our noise analysis is fully comprehensive and, hence, could be applied to any 2D layered systems.

Kwon, Jiseok↗
DOE OSTI2020

A numerical study of particle jetting in a dense particle bed driven by an air-blast

In this work, the particle jetting behavior in a blast-driven dense particle bed is studied at early times. Four-way coupled Euler–Lagrange simulations are performed using a high-order discontinuous Galerkin spectral element solver coupled with a high-order Lagrangian particle solver, wherein the inter-particle collisions are resolved using a discrete element method collision model. Following the experiments of Rodriguez et al. [“Formation of particle jetting in a cylindrical shock tube,” Shock Waves 23(6), 619–634 (2013)] and the simulations of Osnes et al. [“Numerical simulation of particle jet formation induced by shock wave acceleration in a Hele-Shaw cell,” Shock Waves 28(3), 451–461 (2018)], the simulations are performed in a quasi-two-dimensional cylindrical geometry (Hele-Shaw cell). Parametric studies are carried out to assess the impact of the coefficient of restitution and the strength of the incident shock on the particle jetting behavior. The deposition of vorticity through a multiphase (gas–particle) analog of Richtmyer–Meshkov instability is observed to play a crucial role in channeling the particles into well-defined jets at the outer edge of the particle bed. This is confirmed by the presence of vortex pairs around the outer jets. Furthermore, the effect of the relaxation of the relative velocity between the two phases on the vorticity generation is explored by analyzing the correlation between the radial velocity of particles and the radial velocity of the gas at the particle location.

42 ENGINEERING↗
DOE OSTI2020

Raman studies of hydrogen trapped in As 4 O 6 ·2H 2 at high pressure and low temperature

In this work, Raman spectroscopic measurements of the arsenolite–hydrogen inclusion compound As 4 O 6 ·2H 2 were performed in diamond anvil cells at high pressure and variable temperature down to 80 K. The experimental results were complemented by ab initio molecular dynamics simulations and phonon calculations. Observation of three hydrogen vibrons in As 4 O 6 ·2H 2 is reported in the entire temperature and pressure range studied (up to 24 GPa). While the experiments performed with protium and deuterium at variable temperatures allowed for the assignment of two vibrons as Q 1 (1) and Q 1 (0) transitions of ortho and para spin isomers of hydrogen trapped in the inclusion compound, the origin of the third vibron could not be unequivocally established. Low-temperature spectra revealed that the lowest-frequency vibron is actually composed of two overlapping bands of A g and T 2g symmetries dominated by H 2 stretching modes as predicted by our previous density functional theory calculations. We observed low-frequency modes of As 4 O 6 ·2H 2 vibrations dominated by H 2 “librations,” which were missed in a previous study. A low-temperature fine structure was observed for the J = 0 → 2 and J = 1 → 3 manifolds of hydrogen trapped in As 4 O 6 ·2H 2 , indicating the lifting of degeneracy due to an anisotropic environment. A non-spherical distribution was captured by molecular dynamics simulations, which revealed that the trajectory of H 2 molecules is skewed along the crystallographic $\langle$111$\rangle$ direction. Last but not least, low-temperature synchrotron powder x-ray diffraction measurements on As 4 O 6 ·2H 2 revealed that the bulk structure of the compound is preserved down to 5 K at 1.6 GPa.

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

Photoinduced charge transfer in Zn(II) and Au(III)-ligated symmetric and asymmetric bacteriochlorin dyads: A computational study

The excited-state properties and photoinduced charge-transfer (CT) kinetics in a series of symmetrical and asymmetrical Zn- and Au-ligated meso–meso-connected bacteriochlorin (BChl) complexes are studied computationally. BChl derivatives, which are excellent near-IR absorbing chromophores, are found to play a central role in bacterial photosynthetic reaction centers but are rarely used in artificial solar energy harvesting systems. The optical properties of chemically linked BChl complexes can be tuned by varying the linking group and involving different ligated metal ions. We investigate charge transfer in BChl dyads that are either directly linked or through a phenylene ring (1,4- phenylene) and which are ligating Zn or Au ions. The directly linked dyads with a nearly perpendicular arrangement of the BChl units bear markedly different properties than phenylene linked dyads. In addition, we find that the dielectric dependence of the intramolecular CT rate is very strong in neutral Zn-ligated dyads, whereas cationic Au-ligated dyads show negligible dielectric dependence of the CT rate. Rate constants of the photo induced CT process are calculated at the semiclassical Marcus level and are compared to fully quantum mechanical Fermi’s golden rule based values. The rates are calculated using a screened range separated hybrid functional that offers a consistent framework for addressing environment polarization. We study solvated systems in two solvents of a low and a high scalar dielectric constant.

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

In situ TEM study of crystallization and chemical changes in an oxidized uncapped Ge 2 Sb 2 Te 5 film

Ge 2 Sb 2 Te 5 (GST-225) has been the most used active material in nonvolatile phase-change memory devices. Understanding the kinetics and dynamics involved in crystallization is critical for the optimization of materials and devices. A GST-225 thin film of 20 nm thickness was prepared by sputtering directly onto a Protochip and left uncapped and exposed to atmosphere for approximately 1 year. Here, early stages of crystallization and growth of the film have been studied inside the TEM from room temperature to 140 °C. The morphological and structural transformations have been studied by a C s -corrected environmental TEM, and images have been recorded using a high-speed low electron dose camera (Gatan K3 IS). The amorphous to crystalline transformation has been observed at ~35 °C. From the large field, high-resolution images obtained using the Gatan K3 IS camera early crystallization can be detected and nucleation rates and growth velocities can be obtained.

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

On the study of hydrodynamic instabilities in the presence of background magnetic fields in high-energy-density plasmas

Blast-wave-driven hydrodynamic instabilities are studied in the presence of a background B-field through experiments and simulations in the high-energy-density (HED) physics regime. In experiments conducted at the Laboratoire pour l’utilisation des lasers intenses (LULI), a laser-driven shock-tube platform was used to generate a hydrodynamically unstable interface with a prescribed sinusoidal surface perturbation, and short-pulse x-ray radiography was used to characterize the instability growth with and without a 10-T B-field. The LULI experiments were modeled in FLASH using resistive and ideal magnetohydrodynamics (MHD), and comparing the experiments and simulations suggests that the Spitzer model implemented in FLASH is necessary and sufficient for modeling these planar systems. These results suggest insufficient amplification of the seed B-field, due to resistive diffusion, to alter the hydrodynamic behavior. Although the ideal-MHD simulations did not represent the experiments accurately, they suggest that similar HED systems with dynamic plasma-β (=2μ0ρv2/B2) values of less than ∼100 can reduce the growth of blast-wave-driven Rayleigh–Taylor instabilities. These findings validate the resistive-MHD FLASH modeling that is being used to design future experiments for studying B-field effects in HED plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Experimental and theoretical study of energy transfer in a chromophore triad: What makes modeling dynamics successful?

Simulation of electronic dynamics in realistically large molecular systems is a demanding task that has not yet achieved the same level of quantitative prediction already realized for its static counterpart. This is particularly true for processes occurring beyond the Born–Oppenheimer regime. Non-adiabatic molecular dynamics (NAMD) simulations suffer from two convoluted sources of error: numerical algorithms for dynamics and electronic structure calculations. While the former has gained increasing attention, particularly addressing the validity of ad hoc methodologies, the effect of the latter remains relatively unexplored. Indeed, the required accuracy for electronic structure calculations to reach quantitative agreement with experiment in dynamics may be even more strict than that required for static simulations. In this study, we address this issue by modeling the electronic energy transfer in a donor–acceptor–donor (D–A–D) molecular light harvesting system using fewest switches surface hopping NAMD simulations. In the studied system, time-resolved experimental measurements deliver complete information on spectra and energy transfer rates. Subsequent modeling shows that the calculated electronic transition energies are “sufficiently good” to reproduce experimental spectra but produce over an order of magnitude error in simulated dynamical rates. We further perform simulations using artificially shifted energy gaps to investigate the complex relationship between transition energies and modeled dynamics to understand factors affecting non-radiative relaxation and energy transfer rates.

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

Study of vacuum ultraviolet emission in helium and helium/nitrogen mixtures

Helium is frequently used as a working medium for the generation of plasmas and is capable of energetic photon emissions. These energetic photon emissions are often attributed to the formation of helium excimer and subsequent photon emission. When the plasma device is exposed to another gas, such as nitrogen, this energetic photon emission can cause photoionization and further ionization wave penetration into the additional gas. Often ignored are the helium resonance emissions that are assumed to be radiation trapped and therefore not pertinent to photoionization. Here, experimental evidence for the presence of helium atomic emission in a pulsed discharge at ten’s of Torr is shown. Simulations of a discharge in similar conditions agree with the experimental measurements. In this context, the role of atomic and molecular helium light emission on photoionization of molecular nitrogen in an ionization wave is studied using a kinetic modeling approach that accounts for radiation dynamics in a developing low-temperature plasma. Three different mixtures of helium at a total pressure of 250 Torr are studied in simulation. Photoionization of the nitrogen molecule by vacuum ultraviolet helium emission is used as the only seed source ahead of the ionization front. It is found that even though radiation trapped, the atomic helium emission lines are the significant source of photoionization of nitrogen. The significant effect of radiation trapped photon emission on ionization wave dynamics demonstrates the need to consider these radiation dynamics in plasma reactors where self-absorbed radiation is ignored.

42 ENGINEERING↗
DOE OSTI2021

Additively manufactured electrodes for plasma and power-flow studies in high-power transmission lines on the 1-MA MAIZE facility

Power-flow studies on the 30-MA, 100-ns Z facility at Sandia National Laboratories have shown that plasmas in the facility’s magnetically insulated transmission lines (MITLs) and double post-hole convolute can result in a loss of current delivered to the load. To study power-flow physics on the 1-MA, 100-ns MAIZE facility at the University of Michigan, planar MITL loads and planar post-hole convolute loads have been developed that extend into the lines of sight for various imaging diagnostics on MAIZE. These loads use 3D-printed dielectric support structures lined with thin foils of either aluminum or stainless steel. Here, the metal foils serve as the current-carrying power-flow surfaces, which generate plasma during the current pulse. The foil thickness (50 µm) and widths (11.5–16 mm) are selected to ensure a sufficient linear current density (0.5–0.7 MA/cm) for plasma formation. Laser backlighting (532 nm) and visible-light self-emission imaging capture the overall plasma evolution in the anode–cathode gaps, including the gap closure velocities (1–4 cm/μs).

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Demonstration of an x-ray Raman spectroscopy setup to study warm dense carbon at the high energy density instrument of European XFEL

We present a proof-of-principle study demonstrating x-ray Raman Spectroscopy (XRS) from carbon samples at ambient conditions in conjunction with other common diagnostics to study warm dense matter, performed at the high energy density scientific instrument of the European x-ray Free Electron Laser (European XFEL). We obtain sufficient spectral resolution to identify the local structure and chemical bonding of diamond and graphite samples, using highly annealed pyrolytic graphite spectrometers. Due to the high crystal reflectivity and XFEL brightness, we obtain signal strengths that will enable accurate XRS measurements in upcoming pump–probe experiments with a high repetition-rate, where the samples will be pumped with high-power lasers. Molecular dynamics simulations based on density functional theory together with XRS simulations demonstrate the potential of this technique and show predictions for high-energy-density conditions. Our setup allows simultaneous implementation of several different diagnostic methods to reduce ambiguities in the analysis of the experimental results, which, for warm dense matter, often relies on simplifying model assumptions. The promising capabilities demonstrated here provide unprecedented insights into chemical and structural dynamics in warm dense matter states of light elements, including conditions similar to the interiors of planets, low-mass stars, and other celestial bodies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Electrostatic gating of ion transport in carbon nanotube porins: A modeling study

Carbon nanotube porins (CNTPs) are biomimetic membrane channels that demonstrate excellent biocompatibility and unique water and ion transport properties. Gating transport in CNTPs with external voltage could increase control over ion flow and selectivity. Herein, we used continuum modeling to probe the parameters that enable and further affect CNTP gating efficiency, including the size and composition of the supporting lipid membrane, slip flow in the carbon nanotube, and the intrinsic electronic properties of the nanotube. Our results show that the optimal gated CNTP device consists of a semiconducting CNTP inserted into a small membrane patch containing an internally conductive layer. Moreover, we demonstrate that the ionic transport modulated by gate voltages is controlled by the charge distribution along the CNTP under the external gate electric potential. The theoretical understanding developed in this study offers valuable guidance for the design of gated CNTP devices for nanofluidic studies, novel biomimetic membranes, and cellular interfaces in the future.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Impact of particle loading and phase coupling on gas–solid flow dynamics: A case study of a two-phase, gas–solid flow in an annular pipe

The present study is devoted to a two-phase, gas–solid flow in an annular pipe (hollow cylinder) at an elevated pressure of 15 bars and moderate Reynolds number of circa 6000. The influence of the particle loading, the interaction between the phases, and turbulence dispersion on the flow dynamics is systematically studied by means of computational fluid dynamics simulations, employing the Ansys FLUENT commercial package. The cases with a particle volumetric fraction of 1.2% are referred to as “high particle loading,” and those with 0.13% are denoted as “low particle loading.” The following cases are investigated: (1) pure gas flow; (2) low particle loading two-phase flow with one-way coupling and with turbulence dispersion; (3) low particle loading two-phase flow with two-way coupling but without turbulence dispersion; (4) low particle loading two-phase flow with two-way coupling and with turbulence dispersion; (5) high particle loading two-phase flow with one-way coupling and with turbulence dispersion; (6) high particle loading two-phase flow with two-way coupling but without turbulence dispersion; and (7) high particle loading two-phase flow with two-way coupling and with turbulence dispersion. Additionally, the boundary layer is found to grow without fluctuations of the turbulent kinetic energy (TKE) for cases 1, 2, and 5. For case 4, the TKE fluctuations have been identified, although they appear to be less substantial than those in cases 6 and 7. The authors attribute the semi-chaotic nature of the TKE fluctuations to the particle loading and two-way coupling. In addition, the onset and development of the flow instability have been observed at a random axial distance in cases 4, 6, and 7. Such instability is also attributed to the two-way coupling with turbulence dispersion in the flow. It is concluded that the particle loading, one-way, or two-way coupling between the phases, and the turbulence dispersion models significantly influence the development of the flow dynamics with the same inlet and boundary conditions. Consequently, it is not a trivial question, which result a user should trust. The present computational results inspire to perform verification as well as experimental validation of the simulations, so the simulation results can subsequently be used with confidence for design analysis.

42 ENGINEERING↗
DOE OSTI2021

Experimental study of atmospheric pressure single-pulse nanosecond discharge in pin-to-pin configuration

We present an experimental study of nanosecond high-voltage discharges in a pin-to-pin electrode configuration at atmospheric conditions operating in single-pulse mode (no memory effects). Discharge parameters were measured using microwave Rayleigh scattering, laser Rayleigh scattering, optical emission spectroscopy enhanced with a nanosecond probing pulse, and fast photography. Spark and corona discharge regimes were studied for electrode gap sizes 2-10 mm and discharge pulse duration of 90 ns. The spark regime was observed for gaps < 6 mm using discharge pulse energies of 0.6-1 mJ per mm of the gap length. Higher electron number densities, total electron number per gap length, discharge currents, and gas temperatures were observed for smaller electrode gaps and larger pulse energies, reaching maximal values of about 7.5 x 10 15 cm -3 , 3.5 x 10 11 electrons per mm, 22 A, and 4,000 K (at 10 microseconds after the discharge), respectively, for a 2 mm gap and 1 mJ/mm discharge pulse energy. Initial breakdown was followed by a secondary breakdown occurring about 30-70 ns later and was associated with ignition of a cathode spot and transition to cathodic arc. Here, a majority of the discharge pulse energy was deposited into the gas before the secondary breakdown (85-89%). The electron number density after the ns-discharge pulse decayed with a characteristic time scale of 150 ns governed by dissociative recombination and electron attachment to oxygen mechanisms. For the corona regime, substantially lower pulse energies (~0.1 mJ/mm), peak conduction current (1-2 A), and electron numbers (3-5 x 10 10 electrons per mm), and gas temperatures (360 K) were observed.

42 ENGINEERING↗
DOE OSTI2022

Study of self-interaction-errors in barrier heights using locally scaled and Perdew-Zunger self-interaction methods

We study the effect of self-interaction errors on the barrier heights of chemical reactions. For this purpose we use the well-known Perdew-Zunger [J. P. Perdew and A. Zunger, Phys. Rev. B,23, 5048 (1981)] self-interaction-correction(PZSIC), as well two variations of the recently developed, locally scaled self-interaction correction (LSIC) [Zope et al.,J. Chem. Phys.151, 214108 (2019)] to study the barrier heights of the BH76 benchmark dataset. Our results show that both PZSIC and especially the LSIC methods improve the barrier heights relative to the local density approximation(LDA). The version of LSIC that uses the iso-orbital indicator z as a scaling factor gives a more consistent improvement than an alternative version that uses an orbital-dependent factor based on the ratio of orbital densities to the total electron density. We show that LDA energies evaluated using the self-consistent and self-interaction-free PZSIC densities can be used to assess density-driven errors. Furthermore, the LDA reaction barrier errors for the BH76 set are found to contain significant density-driven errors for all types of reactions contained in the set, but the corrections due to adding SIC to the functional are much larger than those stemming from the density for the hydrogen transfer reactions and of roughy equal size for the non-hydrogen transfer reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Double cylinder target design for study of hydrodynamic instabilities in multi-shell ICF

Cylindrical implosions are used to study hydrodynamic instability growth for inertial confinement fusion (ICF) applications, as the cylindrical geometry allows for easier diagnostic access while retaining convergence effects. In this work, we use the established cylindrical implosion platform [Palaniyappan et al., Phys. Plasmas 27, 042708 (2020)] to inform the double shell ICF campaign [Montgomery et al., Phys. Plasmas 25, 092706 (2018)]. We present a design for a double cylindrical target as an analogue to the double shell ICF capsule in order to study hydrodynamic instability growth on the high-Z inner shell. Our design work is done with two-dimensional (2D) Eulerian radiation-hydrodynamics simulations, considering the axial uniformity of the implosion and feasibility of measuring the instability growth of pre-seeded single mode sinusoidal perturbations. We discuss in depth the design for a target to be directly driven at the OMEGA laser facility [Boehly et al., Opt. Commun. 133, 495 (1997)]. We evaluate the design for axial implosion symmetry and visibility of instability growth using synthetic radiographs constructed from the simulations, as the instability growth on the inner cylinder is experimentally measured using x-ray radiography of the implosion. We find that the seeded perturbation growth on the inner cylinder should be visible in an experiment, even with axial implosion asymmetry and preheat. We compare our 2D simulations with linear theory predictions for perturbation growth and show that a cylinder with lower azimuthal mode number (mode-20) perturbations compares more favorably with linear theory, while a cylinder with higher azimuthal mode number (mode-40) perturbations at the same starting amplitude saturates and is over-predicted by linear theory.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗