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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 937 records · Page 52
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Mass density fluctuations in quantum and classical descriptions of liquid water

First principles molecular dynamics simulation protocol is established using revised functional of Perdew-Burke-Ernzerhof (revPBE) in conjunction with Grimme's third generation of dispersion (D3) correction to describe properties of water at ambient conditions. This study also demonstrates the consistency of the structure of water across both isobaric (NpT) and isothermal (NVT) ensembles. Going beyond the standard structural benchmarks for liquid water, we compute properties that are connected to both local structure and mass density fluctuations that are related to concepts of solvation and hydrophobicity. Finally, we directly compare our revPBE results to the Becke-Lee-Yang-Parr (BLYP) plus Grimme dispersion corrections (D2) and both the empirical fixed charged model (SPC/E) and many body interaction potential model (MB-pol) to further our understanding of how the computed properties herein depend on the form of the interaction potential.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Temperature effects on atomic pair distribution functions of melts

Using molecular dynamics simulations, we investigate the temperature-dependent evolution of the first peak position/shape in pair distribution functions of liquids. For metallic liquids, the peak skews towards the left (shorter distance side) with increasing temperature, similar to the previously reported anomalous peak shift. Making use of constant-volume simulations in the absence of thermal expansion and change in inherent structure, we demonstrate that the apparent shift of the peak maximum can be a result of the asymmetric shape of the peak, as the asymmetry increases with temperature-induced spreading of neighboring atoms to shorter and longer distances due to the anharmonic nature of the interatomic interaction potential. These findings shed light on the first-shell expansion/contraction paradox for metallic liquids, aside from possible changes in local topological or chemical short-range ordering. The melts of covalent materials are found to exhibit an opposite trend of peak shift, which is attributed to an effect of the directionality of the interatomic bonds.

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

Ultrafast vibrational dynamics of a trigonal planar anionic probe in ionic liquids (ILs): A two-dimensional infrared (2DIR) spectroscopic investigation

A major impediment limiting the widespread application of ionic liquids (ILs) is their high shear viscosity. Incorporation of a tricyanomethanide (TCM - ) anion in ILs leads to low shear viscosity and improvement of several characteristics suitable for large scale applications. However, properties including interactions of TCM - with the local environment and dynamics of TCM - have not been thoroughly investigated. Herein, we have studied the ultrafast dynamics of TCM - in several imidazolium ILs using linear IR and two-dimensional infrared spectroscopy techniques. The spectral diffusion dynamics of the CN stretching modes of TCM - in all ILs exhibit a nonexponential behavior with a short time component of ~2 ps and a long time component spanning ~9 ps to 14 ps. The TCM - vibrational probe reports a significantly faster relaxation of ILs compared to those observed previously using linear vibrational probes, such as thiocyanate and selenocyanate. Our results indicate a rapid relaxation of the local ion-cage structure embedding the vibrational probe in the ILs. The faster relaxation suggests that the lifetime of the local ion-cage structure decreases in the presence of TCM - in the ILs. Linear IR spectroscopic results show that the hydrogen-bonding interaction between TCM - and imidazolium cations in ILs is much weaker. Shorter ion-cage lifetimes together with weaker hydrogen-bonding interactions account for the low shear viscosity of TCM - based ILs compared to commonly used ILs. In addition, this work demonstrates that TCM - can be used as a potential vibrational reporter to study the structure and dynamics of ILs and other molecular systems.

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

Atomistic simulations of the thermal conductivity of liquids

We present a method based on sinusoidal approach to equilibrium molecular dynamics (SAEMD) to compute the thermal conductivity of liquids Similar to nonequilibrium molecular dynamics, and unlike equilibrium simulations based on the Green-Kubo formalism, the method only requires the calculation of forces and total energies. The evaluation of heat fluxes and energy densities is not necessary, thus offering the promise of efficiently implementing first principles simulations based on density functional theory or deep molecular dynamics. Our approach is a generalization of SAEMD for solids, where the thermal conductivity is computed in the steady state, instead of a transient regime, thus properly taking into account diffusive terms in the heat equation. We present results for liquid water at ambient conditions and under pressure and discuss simulation requirements to obtain converged values of the thermal conductivity as a function of size and simulation time.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Linking density functional and mode coupling models for supercooled liquids

We compare predictions from two familiar models of the metastable supercooled liquid, respectively, constructed with thermodynamic and dynamic approaches. In the so called density functional theory the free energy F[ρ] of the liquid is a functional of the inhomogeneous density ρ(r). The metastable state is identified as a local minimum of F[ρ]. The sharp density profile characterizing ρ(r) is identified as a single particle oscillator, whose frequency is obtained from the parameters of the optimum density function. On the other hand, a dynamic approach to supercooled liquids is taken in the mode coupling theory (MCT) which predict a sharp ergodicity-non-ergodicity transition at a critical density. The single particle dynamics in the non-ergodic state, treated approximately, represents a propagating mode whose characteristic frequency is computed from the corresponding memory function of the MCT. The mass localization parameters in the above two models (treated in their simplest forms) are obtained, respectively, in terms of the corresponding natural frequencies depicted and are shown to have comparable magnitudes.

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

Conductivity and Transference Numbers in Lithium Salt-Doped Block Copolymeric Ionic Liquid Electrolytes

We present multiscale molecular dynamics simulation results comparing the conductivity and transference numbers in lithium salt-doped polymeric ionic liquids (PolyILs) and the lamellar phases of block copolymeric ionic liquids (coPolyILs). In both systems, the anion mobilities decreased with salt loading. Lithium ions exhibited negative mobilities in both systems, but the magnitudes decreased with an increase in salt concentrations. More interestingly, the anion mobilities were lower in the lamellar systems compared to homopolymers in magnitude, but the lithium ion mobilities and transference numbers were less negative in such systems. We examine the anion–cation and lithium–anion interactions in terms of radial distribution functions, coordination characteristics, and ion-pair relaxation timescales. Based on such analyses, we rationalize the salt concentration dependencies as a result of the interfacial interactions in lamellar systems and the competition between anion–cation and lithium–anion interactions in both PolyILs and coPolyILs. Altogether, the findings presented in this study demonstrate that the modified anion–cation and lithium–anion interactions in the microphase-separated coPolyILs may provide a strategy for realizing higher lithium ion transference numbers relative to the homopolymeric counterparts.

36 MATERIALS SCIENCE↗
DOE OSTI2014

A comparison of molecular dynamics and diffuse interface model predictions of Lennard-Jones fluid evaporation

The unsteady evaporation of a thin planar liquid film is studied by molecular dynamics simulations of Lennard-Jones fluid. The obtained results are compared with the predictions of a diffuse interface model in which capillary Korteweg contributions are added to hydrodynamic equations, in order to obtain a unified description of the liquid bulk, liquid-vapor interface and vapor region. Particular care has been taken in constructing a diffuse interface model matching the thermodynamic and transport properties of the Lennard-Jones fluid. The comparison of diffuse interface model and molecular dynamics results shows that, although good agreement is obtained in equilibrium conditions, remarkable deviations of diffuse interface model predictions from the reference molecular dynamics results are observed in the simulation of liquid film evaporation. It is also observed that molecular dynamics results are in good agreement with preliminary results obtained from a composite model which describes the liquid film by a standard hydrodynamic model and the vapor by the Boltzmann equation. The two mathematical model models are connected by kinetic boundary conditions assuming unit evaporation coefficient.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Polar liquids at charged interfaces: A dipolar shell theory

The structure of polar liquids and electrolytic solutions, such as water and aqueous electrolytes, at interfaces underlies numerous phenomena in physics, chemistry, biology, and engineering. In this work, we develop a continuum theory that captures the essential features of dielectric screening by polar liquids at charged interfaces, including decaying spatial oscillations in charge and mass, starting from the molecular properties of the solvent. The theory predicts an anisotropic dielectric tensor of interfacial polar liquids previously studied in molecular dynamics simulations. We explore the effect of the interfacial polar liquid properties on the capacitance of the electrode/electrolyte interface and on hydration forces between two plane-parallel polarized surfaces. In the linear response approximation, we obtain simple formulas for the characteristic decay lengths of molecular and ionic profiles at the interface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1976

Experiments on the properties of superfluid helium in zero gravity

The paper describes a research program designed to study the behavior of superfluid liquid helium in low and zero gravity in order to determine the properties which are critically important to its use as a stored cryogen for cooling scientific instruments aboard spacecraft for periods up to several months. The experiment program consists of a series of flights of an experiment package on a free-fall trajectory both on an aircraft and on a rocket. The objectives are to study thickness of thin films of helium as a function of acceleration, heat transfer in thin films, heat transfer across copper-liquid helium interfaces, fluid dynamics of bulk helium in high and low accelerations and under various conditions of rotations, alternate methods of separation of liquid and vapor phases and of efficient venting of the vapor, and undesirable thermomechanical oscillations in the vent pipes. Preliminary results from aircraft tests are discussed.

Mason, P.↗
DOE OSTI2016

A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum

A pulsed laser heating system has been developed that enables investigations of the dynamics and kinetics of nanoscale liquid films and liquid/solid interfaces on the nanosecond timescale in ultrahigh vacuum (UHV). Details of the design, implementation and characterization of a nanosecond pulsed laser system for transiently heating nanoscale films are described herein. Nanosecond pulses from a Nd:YAG laser are used to rapidly heat thin films of adsorbed water or other volatile materials on a clean, well-characterized Pt(111) crystal in UHV. Heating rates of ~1010 K/s for temperature increases of ~100 – 200 K are obtained. Subsequent rapid cooling (~5 × 109 K/s) quenches the film, permitting in-situ, post-mortem analysis using a variety of surface science techniques. Lateral variations in the laser pulse energy are ~ ± 3% leading to a temperature uncertainty of ~ ± 5 K for a temperature jump of 200 K. Initial experiments with the apparatus demonstrate that crystalline ice films initially held at 90 K can be rapidly transformed into liquid water films with T > 273 K. No discernable recrystallization occurs during the rapid cooling back to cryogenic temperatures. In contrast, amorphous solid water films heated below the melting point rapidly crystallize. The nanosecond pulsed laser heating system can prepare nanoscale liquid and supercooled liquid films that persist for nanoseconds per heat pulse in an UHV environment, enabling experimental studies of a wide range of phenomena in liquids and at liquid/solid interfaces.

47 OTHER INSTRUMENTATION↗
DOE OSTI2015

Weak links between fast mobility and local structure in molecular and atomic liquids

We investigate by molecular-dynamics simulations, the fast mobility—the rattling amplitude of the particles temporarily trapped by the cage of the neighbors—in mildly supercooled states of dense molecular (linear trimers) and atomic (binary mixtures) liquids. The mixture particles interact by the Lennard-Jones potential. The non-bonded particles of the molecular system are coupled by the more general Mie potential with variable repulsive and attractive exponents in a range which is a characteristic of small n-alkanes and n-alcohols. Possible links between the fast mobility and the geometry of the cage (size and shape) are searched. The correlations on a per-particle basis are rather weak. Instead, if one groups either the particles in fast-mobility subsets or the cages in geometric subsets, the increase of the fast mobility with both the size and the asphericity of the cage is revealed. The observed correlations are weak and differ in states with equal relaxation time. Local forces between a tagged particle and the first-neighbour shell do not correlate with the fast mobility in the molecular liquid. It is concluded that the cage geometry alone is unable to provide a microscopic interpretation of the known, universal link between the fast mobility and the slow structural relaxation. We suggest that the particle fast dynamics is affected by regions beyond the first neighbours, thus supporting the presence of collective, extended fast modes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Nanosecond Lipid Dynamics in Membranes Containing Cholesterol

Lipid dynamics in the cholesterol-rich (40 mol%) liquid-ordered (lo) phase of dimyristoylphosphatidylcholine membranes were studied using neutron spin-echo and neutron backscattering. Recent theoretical and experimental evidence supports the notion of the liquid-ordered phase in phospholipid membranes as a locally structured liquid, with small ordered domains of a highly dynamic nature in equilibrium with a disordered matrix [S. Meinhardt, R. L. C. Vink and F. Schmid, Proc. Natl. Acad. Sci. U. S. A., 2013, 110(12), 4476 4481, C. L. Armstrong et al., PLoS One, 2013, 8(6), e66162]. This local structure was found to have a pronounced impact on the membranes' dynamical properties. We found that the long-wavelength dynamics in the liquid-ordered phase, associated with the elastic properties of the membranes, were faster by two orders of magnitude as compared to the liquid disordered phase. At the same time, collective nanoscale diffusion was significantly slower. The presence of a soft-mode (a slowing down) in the longwavelength dispersion relationship suggests an upper size limit for the ordered lipid domain of ~220 A. Moreover, from the relaxation rate of the collective lipid diffusion of lipid lipid distances, the lifetime of these domains was estimated to be about 100 nanoseconds.

Armstrong, Clare L↗
NASA NTRS1972

Coupling between structure and liquids in a parallel stage space shuttle design

A study was conducted to determine the influence of liquid propellants on the dynamic loads for space shuttle vehicles. A parallel-stage configuration model was designed and tested to determine the influence of liquid propellants on coupled natural modes. A forty degree-of-freedom analytical model was also developed for predicting these modes. Currently available analytical models were used to represent the liquid contributions, even though coupled longitudinal and lateral motions are present in such a complex structure. Agreement between the results was found in the lower few modes.

Kana, D. D.↗
NASA NTRS1972

Coupling between structure and liquid propellants in a parallel-stage space shuttle design.

A study was conducted to determine the influence of liquid propellants on the dynamic loads for space shuttle vehicles. A parallel-stage configuration model was designed and tested to determine the influence of liquid propellants on coupled natural modes. A forty degree-of-freedom analytical model was also developed for predicting these modes. Currently available analytical models were used to represent the liquid contributions, even though coupled longitudinal and lateral motions are present in such a complex structure. Agreement between the results was found in the lower few modes.

Kana, D. D.↗
DOE OSTI2016

Atomistic modelling of evaporation and explosive boiling of thin film liquid argon over internally recessed nanostructured surface

Molecular dynamics (MD) simulations have been carried out to investigate evaporation and explosive boiling phenomena of thin film liquid argon on nanostructured solid surface with emphasis on the effect of solid-liquid interfacial wettability. The nanostructured surface considered herein consists of trapezoidal internal recesses of the solid platinum wall. The wetting conditions of the solid surface were assumed such that it covers both the hydrophilic and hydrophobic conditions and hence effect of interfacial wettability on resulting evaporation and boiling phenomena was the main focus of this study. The initial configuration of the simulation domain comprised of a three phase system (solid platinum, liquid argon and vapor argon) on which equilibrium molecular dynamics (EMD) was performed to reach equilibrium state at 90 K. After equilibrium of the three-phase system was established, the wall was set to different temperatures (130 K and 250 K for the case of evaporation and explosive boiling respectively) to perform non-equilibrium molecular dynamics (NEMD). The variation of temperature and density as well as the variation of system pressure with respect to time were closely monitored for each case. The heat flux normal to the solid surface was also calculated to illustrate the effectiveness of heat transfer for hydrophilic and hydrophobic surfaces in cases of both nanostructured surface and flat surface. The results obtained show that both the wetting condition of the surface and the presence of internal recesses have significant effect on normal evaporation and explosive boiling of the thin liquid film. The heat transfer from solid to liquid in cases of surface with recesses are higher compared to flat surface without recesses. Also the surface with higher wettability (hydrophilic) provides more favorable conditions for boiling than the low-wetting surface (hydrophobic) and therefore, liquid argon responds quickly and shifts from liquid to vapor phase faster in case of hydrophilic surface. The heat transfer rate is also much higher in case of hydrophilic surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Intermolecular correlations of liquid and glassy CS 2 studied by synchrotron radiation x-ray diffraction

How is the orientation of molecular liquids ordered on cooling? What are the basic structures of molecular glasses, e.g., close to the crystalline structure or some special structures such as icosahedral cluster? These are long-standing questions in liquid and glass physics. Here, we have constructed a novel cryostat to prepare simple molecular glasses by vapor deposition and performed in situ synchrotron radiation x-ray diffraction experiments. The glassy state of a simple molecule CS 2 , which cannot be vitrified by normal liquid quenching, was successfully prepared with this instrument, and its diffraction data were collected in a wide Q-range of 0.16–25.7 Å -1 with a high-energy diffractometer at BL04B2, SPring-8. The diffraction data of liquid CS 2 were also recorded in a wide temperature range of 160–300 K. These diffraction data were analyzed with molecular dynamics simulations and reverse Monte Carlo modelings to investigate orientational correlation. From the obtained 3D structure models, the orientational correlation between neighboring CS 2 molecules was investigated quantitatively as a function of temperature. At room temperature, the parallel and T-shaped arrangements are preferred for the nearest neighbor correlation. On cooling, these arrangements are developed gradually, and its rate became prominent below the melting temperature (162 K). In the glassy state, the slipped-parallel arrangement is dominant as well as the T-shaped arrangement. Both arrangements appear in the CS 2 crystal, indicating that the structure of glassy CS 2 is close to that of crystalline CS 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Communication: Dynamical and structural analyses of solid hydrogen under vapor pressure

Nuclear quantum effects play a dominant role in determining the phase diagram of H{sub 2}. With a recently developed quantum molecular dynamics simulation method, we examine dynamical and structural characters of solid H{sub 2} under vapor pressure, demonstrating the difference from liquid and high-pressure solid H{sub 2}. While stable hexagonal close-packed lattice structures are reproduced with reasonable lattice phonon frequencies, the most stable adjacent configuration exhibits a zigzag structure, in contrast with the T-shape liquid configuration. The periodic angular distributions of H{sub 2} molecules indicate that molecules are not a completely free rotor in the vapor-pressure solid reflecting asymmetric potentials from surrounding molecules on adjacent lattice sites. Discrete jumps of librational and H–H vibrational frequencies as well as H–H bond length caused by structural rearrangements under vapor pressure effectively discriminate the liquid and solid phases. The obtained dynamical and structural information of the vapor-pressure H{sub 2} solid will be useful in monitoring thermodynamic states of condensed hydrogens.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗