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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

High-Performance First-Principles Molecular Dynamics for Predictive Theory and Modeling

This project focused on developing high-performance software tools for First-Principles Molecular Dynamics (FPMD) simulations, and applying them in investigations of materials relevant to energy conversion processes. FPMD is an atomistic simulation method that combines a quantum-mechanical description of electronic structure with the statistical description provided by molecular dynamics (MD) simulations. This reliance on fundamental principles allows FPMD simulations to provide a consistent description of structural, dynamical and electronic properties of a material. This is particularly useful in systems for which reliable empirical models are lacking. FPMD simulations are increasingly used as a predictive tool for applications such as batteries, solar energy conversion, light-emitting devices, electro-chemical energy conversion devices and other materials. During the course of the project, several new features were developed and added to the open-source Qbox FPMD code. The code was further optimized for scalable operation of large-scale, Leadership-Class DOE computers. When combined with Many-Body Perturbation Theory (MBPT) calculations, this infrastructure was used to investigate structural and electronic properties of liquid water, ice, aqueous solutions, nanoparticles and solid-liquid interfaces. Computing both ionic trajectories and electronic structure in a consistent manner enabled the simulation of several spectroscopic properties, such as Raman spectra, infrared spectra, and sum-frequency generation spectra. The accuracy of the approximations used allowed for direct comparisons of results with experimental data such as optical spectra, X-ray and neutron diffraction spectra. The software infrastructure developed in this project, as applied to various investigations of solids, liquids and interfaces, demonstrates that FPMD simulations can provide a detailed, atomic-scale picture of structural, vibrational and electronic properties of complex systems relevant to energy conversion devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

From bulk to surface: Structure and dynamics of amorphous alumina from deep potential molecular dynamics

Understanding the atomic-scale structure and dynamics of amorphous oxide surfaces is essential for interpreting their chemical reactivity, mechanical stability, and interfacial behavior, yet direct experimental characterization remains challenging. We employ Deep Potential (DP) molecular dynamics to generate large-scale, ab initio -quality models of amorphous Al 2 O 3 bulk glasses and melt-quenched free surfaces, enabling a quantitative analysis of both structure and relaxation dynamics with statistical confidence inaccessible to direct ab initio simulation. The trained DP model reproduces experimental liquid and glass structure, captures the cooling-rate dependence of the bulk glass transition, and corrects systematic biases in the polyhedral populations predicted by widely used classical force fields. At the free surface, mass density recovers to bulk values over ~10 Å, while local coordination requires a slightly wider subsurface region to fully converge. The outermost layer is oxygen-enriched, exhibits altered polyhedral connectivity with contracted Al–O bonds, and hosts a broad population of under-coordinated motifs (notably AlO 3 and OAl 2 ) whose abundances are governed by glass stability. These under-coordinated surface motifs exhibit distinct vibrational signatures and occur as locally paired Lewis acid and Brønsted base sites consistent with bond-valence compensation, yet remain spatially dispersed rather than aggregating into extended clusters. Despite this pronounced structural heterogeneity, surface relaxation and the glass-transition temperature remain comparable to their bulk counterparts, suggesting that the disordered surface is kinetically stable once formed. Together, these results establish a molecular-level picture of amorphous alumina surfaces and demonstrate the capability of machine-learned potentials to resolve structure–property relationships in disordered oxide interfaces.

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

Molecular dynamics simulations of the structure and single-particle dynamics of mixtures of divalent salts and ionic liquids

We report a molecular dynamics study of the structure and single-particle dynamics of mixtures of a protic (ethylammonium nitrate) and an aprotic (1-butyl-3-methylimidazolium hexaflurophosphate [BMIM][PF{sub 6}]) room-temperature ionic liquids doped with magnesium and calcium salts with a common anion at 298.15 K and 1 atm. The solvation of these divalent cations in dense ionic environments is analyzed by means of apparent molar volumes of the mixtures, radial distribution functions, and coordination numbers. For the protic mixtures, the effect of salt concentration on the network of hydrogen bonds is also considered. Moreover, single-particle dynamics of the salt cations is studied by means of their velocity autocorrelation functions and vibrational densities of states, explicitly analyzing the influence of salt concentration, and cation charge and mass on these magnitudes. The effect of the valency of the salt cation on these properties is considered comparing the results with those for the corresponding mixtures with lithium salts. We found that the main structural and dynamic features of the local solvation of divalent cations in ionic liquids are similar to those of monovalent salts, with cations being localized in the polar nanoregions of the bulk mixture coordinated in monodentate and bidentate coordination modes by the [NO{sub 3}]{sup −} and [PF{sub 6}]{sup −} anions. However, stronger electrostatic correlations of these polar nanoregions than in mixtures with salts with monovalent cations are found. The vibrational modes of the ionic liquid (IL) are seen to be scarcely affected by the addition of the salt, and the effect of mass and charge on the vibrational densities of states of the dissolved cations is reported. Cation mass is seen to exert a deeper influence than charge on the low-frequency vibrational spectra, giving a red shift of the vibrational modes and a virtual suppression of the higher energy vibrational modes for the heavier Ca{sup 2+} cations. No qualitative difference with monovalent cations was found in what solvation is concerned, which suggests that no enhanced reduction of the mobility of these cations and their complexes in ILs respective to those of monovalent cations is to be expected.

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

Assessment of Precipitating Marine Stratocumulus Clouds in the E3SMv1 Atmosphere Model: A Case Study from the ARM MAGIC Field Campaign

This paper presents a process-oriented evaluation of precipitating stratocumulus and its transition to cumulus in version 1 of the Energy Exascale Earth System Model (E3SMv1) using comprehensive case-study observations from a field campaign of the Atmospheric Radiation Measurement program (ARM). The E3SMv1 single-column model (SCM) of the marine boundary layer and its low clouds and precipitation are compared to observations including subcloud drizzle retrievals from a combination of Doppler radar and lidar backscatter measurements. Additionally, the SCM is also compared to a large-eddy simulation (LES) of the same case. The combination of advanced remote sensing observations and LES is a powerful framework to evaluate the physical parameterizations of large-scale models. Given the observed large-scale environment, the E3SMv1 SCM realistically represents the evolution of clouds and boundary layer structure during the stratocumulus-to-cumulus transition. The model well simulates the liquid water path and its diurnal cycle in the stratocumulus period as well as the two-layer vertical thermodynamic structure and lower cloud fraction in the transition period. E3SMv1’s success in simulating the cloud in the stratocumulus period permitted examination of its precipitation processes. Here problems were identified with E3SMv1 producing an unrealistically small subcloud precipitation fraction, an unrealistic double peak in the vertical profiles of precipitation mass, and drizzle that evaporates too close to the surface. Further model diagnostics determined that these unrealistic characteristics resulted from an overly long microphysics time step and an unrealistic parameterization of the precipitation fraction. These results imply that careful consideration of these issues is needed in order to better simulate precipitation processes in marine stratocumulus.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Liquid li structure and dynamics: A comparison between OFDFT and second nearest-neighbor embedded-atom method

The structure and dynamics of liquid lithium are studied using two simulation methods: orbital-free (OF) first-principles molecular dynamics (MD), which employs OF density functional theory (DFT), and classical MD utilizing a second nearest-neighbor embedded-atom method potential. The properties we studied include the dynamic structure factor, the self-diffusion coefficient, the dispersion relation, the viscosity, and the bond angle distribution function. Our simulation results were compared to available experimental data when possible. Each method has distinct advantages and disadvantages. For example, OFDFT gives better agreement with experimental dynamic structure factors, yet is more computationally demanding than classical simulations. Classical simulations can access a broader temperature range and longer time scales. The combination of first-principles and classical simulations is a powerful tool for studying properties of liquid lithium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Solvation structures of water in trihexyltetradecylphosphonium-orthoborate ionic liquids

Atomistic molecular dynamics simulations have been performed to investigate effective interactions of isolated water molecules dispersed in trihexyltetradecylphosphonium-orthoborate ionic liquids (ILs). The intrinsic free energy changes in solvating one water molecule from gas phase into bulk IL matrices were estimated as a function of temperature, and thereafter, the calculations of potential of mean force between two dispersed water molecules within different IL matrices were performed using umbrella sampling simulations. The systematic analyses of local ionic microstructures, orientational preferences, probability and spatial distributions of dispersed water molecules around neighboring ionic species indicate their preferential coordinations to central polar segments in orthoborate anions. The effective interactions between two dispersed water molecules are partially or totally screened as their separation distance increases due to interference of ionic species in between. These computational results connect microscopic anionic structures with macroscopically and experimentally observed difficulty in completely removing water from synthesized IL samples and suggest that the introduction of hydrophobic groups to central polar segments and the formation of conjugated ionic structures in orthoborate anions can effectively reduce residual water content in the corresponding IL samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Molecular-Level Insights into the Influence of Ionic Liquids on the Structure and Dynamics of Neutral and Charged Polyimides

We use all-atom molecular dynamics simulations to investigate how increasing ionic functionalization influences polyimide (PI) behavior in ionic liquid (IL) solvation environments. Here, we examine three polymer systems with varying charge densities: a neutral polyimide [N−PI] containing imidazole rings and progressively introduce charge through quaternization to create singly [C−PI] + and doubly charged [C−2PI] 2+ variants across a wide range of IL concentration (0−90 wt %). Through comprehensive structural, mechanical, and electrostatic analyses, we reveal that polymer charge density plays a central role in shaping IL organization and interaction with the polymer matrix. At low IL content, charged systems exhibit strong electrostatic complexation, leading to chain compaction, localized ESP environments, and elevated dielectric constants. As IL concentration increases, the effect of the different polymer charge states becomes less significant. Notably, an intermediate composition regime at approximately 50 wt % IL is associated with changes in IL-rich domain connectivity and overall system behavior across all three PI systems.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Interference of electrical double layers: Confinement effects on structure, dynamics, and screening of ionic liquids

Ionic liquids are widely used as electrolytes in electronic devices in which they are subject to nanoconfinement within nanopores or nanofilms. Because the intrinsic width of an electrical double layer is on the order of several nanometers, nanoconfinement is expected to fundamentally alter the double layer properties. Furthermore, in confined systems, a large portion of the ions are interfacial, e.g., at the electrode interface, leading to significant deviations of electrostatic screening and ion dynamics as compared to bulk properties. In this article, we systematically investigate the interference between electrical double layers for nanoconfined ionic liquids and the resulting influence on the structure, dynamics, and screening behavior. We perform molecular dynamics simulations for the ionic liquids [BMIm + ][BF$^-_4$] and [BMIm + ][PF$^-_6$] confined between two flat electrodes at systematic separation distances between 1.5 nm and 4.5 nm for both conducting and insulating boundary conditions. We find that while ion dynamics is expectedly slower than in the bulk (by ~2 orders of magnitude), there is an unexpected non-linear trend with the confinement length that leads to a local maximum in dynamic rates at ~3.5–4.5 nm confinement. We show that this nonlinear trend is due to the ion correlation that arises from the interference between opposite double layers. We further evaluate confinement effects on the ion structure and capacitance and investigate the influence of electronic polarization of the ionic liquid on the resulting properties. This systematic evaluation of the connection between electrostatic screening and structure and dynamics of ionic liquids in confined systems is important for the fundamental understanding of electrochemical supercapacitors.

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

A high-dimensional neural network potential for molecular dynamics simulations of condensed phase nickel and phase transitions

A high-dimensional neural network interatomic potential was developed and used in molecular dynamics simulations of condensed phase Ni and Ni systems with liquid–solid phase coexistence. The reference data set was generated by sampling the potential energy surface over a broad temperature-pressure domain using ab initio MD simulations to train a unified potential. Excellent agreement was achieved between bulk face-centered cubic nickel thermal expansion simulations and relevant experimental data. The same potential also yields accurate structures and diffusivities in the liquid state. The phase transition between liquid and solid phases was simulated using the two-phase interface method. The predicted melting point temperature is within a few kelvins of the literature value. Here, the general methodology could be applied to describe crystals with much more complex phase behaviors.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2013

Final Technical Report: SISGR: The Influence of Electrolyte Structure and Electrode Morphology on the Performance of Ionic-Liquid Based Supercapacitors: A Combined Experimental and Simulation Study

Obtaining fundamental understanding and developing predictive modeling capabilities of electrochemical interfaces can significantly shorten the development cycles of electrical double layer capacitors (EDLCs). A notable improvement in EDLC performance has been achieved due to recent advances in understanding charge storage mechanisms, development of advanced nanostructured electrodes and electrochemically stable electrolytes. The development of new generation of EDLCs is intimately linked to that of nanostructured carbon materials which have large surface area, good adsorption/desorption properties, good electrical conductivity and are relatively inexpensive. To address these scientific challenges the efforts of an interdisciplinary team of modelers and experimentalists were combined to enhance our understanding of molecular level mechanisms controlling the performance of EDLCs comprised of room temperature ionic liquid (RTIL) electrolytes and nanostructured carbon-based electrodes and to utilize these knowledge in the design of a new generation of materials and devices for this energy storage application. Specifically our team efforts included: atomistic molecular dynamics simulations, materials science and electrode/device assembly, and synthesis and characterization of RTIL electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2019

Temperature-Dependent Structural Evolution in Au 44 Ga 56 Liquid Eutectic Alloy

We report that temperature-dependent short-range structural evolution of Au 44 Ga 56 liquid eutectic alloy has been studied by in situ extended X-ray absorption fine structure (EXAFS), in situ high-energy X-ray diffraction (HEXRD) together with first-principles molecular dynamics (FPMD) simulations. It is found that the short-range structure of Au 44 Ga 56 liquid strongly inherits the local atomic packing of the AuGa compound. A short-range structural change in Ga-centered clusters is revealed by in situ EXAFS data at the Ga K-edge at about 970 K, while no such change in Au-centered clusters appears at the Au L-III-edge. The in situ HEXRD and FPMD simulations also confirm the existence of a liquid-to-liquid crossover (LLC) in the Au 44 Ga 56 liquid at a temperature range of about 1000-1100 K, mainly lying in the local structural change around Ga atoms. Indeed, the alloys quenched from the liquid phases below 1000 K and above 1100 K exhibit differences in structure and magnetic properties, which opens a possibility to fabricate new materials with different structures and properties in LLC-containing alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2020

CP2K: An Electronic Structure and Molecular Dynamics Software Package - Quickstep: Efficient and Accurate Electronic Structure Calculations

CP2K is an open source electronic structure and molecular dynamics software package to perform atomistic simulations of solid-state, liquid, molecular and biological systems. It is especially aimed at massively-parallel and linear-scaling electronic structure methods and state-of-the-art ab-initio molecular dynamics simulations. Excellent performance for electronic structure calculations is achieved using novel algorithms implemented for modern high-performance computing systems. This review revisits the main capabilities of CP2K to perform efficient and accurate electronic structure simulations. The emphasis is put on density functional theory and multiple post-Hartree-Fock methods using the Gaussian and plane wave approach and its augmented all-electron extension. TDK has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No. 716142). VRR has been supported by the Swiss National Science Foundation in the form of Ambizione grant No. PZ00P2 174227 and RZK by the Natural Sciences and Engineering Research Council of Canada (NSERC) through Discovery Grants (RGPIN-2016-0505). GKS and CJM are supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. UK based work was funded under the embedded CSE programme of the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk), grants eCSE03-011, eCSE06-6, eCSE08-9, eCSE13-17 and the EPSRC (EP/P022235/1) grant “Surface and Interface Toolkit for the Materials Chemistry Community". Computational resources were provided by the Swiss National Supercomputing Centre (CSCS) and Compute Canada. The generous allocation of computing time on the FPGA-based supercomputer “Noctua" at PC2 is kindly acknowledged.

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

The nucleation process and the roles of structure and density fluctuations in supercooled liquid Fe

We observed homogeneous nucleation process of supercooled liquid Fe by molecular dynamics simulations. Using bond-orientational order parameters together with Voronoi polyhedron method, we characterized local structure, calculated the volume of Voronoi polyhedra of atoms and identified the structure and density fluctuations. We monitored the formation of nucleus and analyzed its inner structure. The birth and growth of the pre-nucleus and nucleus are accompanied with aggregating and disaggregating processes in the time scale of femtosecond. Only the initial solid-like clusters (ISLC), ranging from 1 to 7 atoms, pop up directly from liquid. The relation between the logarithm of number of clusters and the cluster size was found to be linear for ISLCs and was observed to be parabolic for all solid-like clusters (SLC) due to aggregating and disaggregating effects. The nucleus and pre-nuclei mainly consist of body centered cubic (BCC) and hexagonal close packed atoms, while the BCC atoms tend to be located at the surface. Medium-range structure fluctuations induce the birth of ISLCs, benefit the aggregation of embryos and remarkably promote the nucleation. But density fluctuations contribute little to nucleation. The lifetime of most icosahedral-like atoms (ICO) is shorter than 0.7 ps. No obvious relationship was found between structure/density fluctuations and the appearance of ICO atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Stokes–Einstein relation and excess entropy in Al-rich Al-Cu melts

We investigate the conditions for the validity of the Stokes-Einstein relation that connects diffusivity to viscosity in melts using entropy-scaling relationships developed by Rosenfeld. Employing ab initio molecular dynamics simulations to determine transport and structural properties of liquid Al{sub 1−x}Cu{sub x} alloys (with composition x ≤ 0.4), we first show that reduced self-diffusion coefficients and viscosities, according to Rosenfeld's formulation, scale with the two-body approximation of the excess entropy except the reduced viscosity for x = 0.4. Then, we use our findings to evidence that the Stokes-Einstein relation using effective atomic radii is not valid in these alloys while its validity can be related to the temperature dependence of the partial pair-excess entropies of both components. Finally, we derive a relation between the ratio of the self-diffusivities of the components and the ratio of their pair excess entropies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Molecular dynamics simulation studies of structural and dynamical properties of rapidly quenched Al

The structural and dynamical properties of rapidly quenched Al are studied by molecular dynamics simulations. The pair-correlation function of high temperature liquid Al agrees well with the experimental results. Different cooling rates are applied with high cooling rates leading to glass formation, while low cooling rates leading to crystallization. The local structures are characterized by Honeycutt–Andersen indices and Voronoi tessellation analysis. The results show that for high cooling rates, the local structures of the liquid and glassy Al are predominated by icosahedral clusters, together with considerable amount of face-centered cubic and hexagonal close packed short-range orders. These short-range order results are further confirmed using the recently developed atomic cluster alignment method. Moreover, the atomic cluster alignment clearly shows the crystal nucleation process in supercooled liquid of Al. Finally, the mean square displacement for the liquid is also analyzed, and the corresponding diffusion coefficient as a function of temperature is calculated.

36 MATERIALS SCIENCE↗