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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 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Reactive molecular dynamics models from ab initio molecular dynamics data using relative entropy minimization

Here, we present two new multiscale molecular dynamics (MS-RMD) models for the hydrated excess proton in water developed directly from ab initio molecular dynamics (AIMD) simulation data of the same system. The potential of mean force along the proton transfer reaction coordinate and radial distribution functions for the MS-RMD models are shown faithfully reproduce those of AIMD. The models are developed using an algorithm based on relative entropy minimization, thus demonstrating the ability of the method to rapidly generate accurate and highly efficient reactive MD force fields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Bergman-type medium range order in amorphous Zr77Rh23 alloy studied by ab initio molecular dynamics simulations

In recent years, some arguments about the existence of medium-range order (MRO) in the Zr-Rh system have been put forward. However, research on the structural features of the Zr-Rh binary alloy at the atomic level is still lacking. This study uses ab initio molecular dynamics simulations to systematically study the local structures of Zr77Rh23 from the liquid to the glassy states. Pair correlation function (PCF), coordination number (CN), Honeycutt–Anderson(HA) index, bond-angle distribution functions, and the Voronoi tessellation method are used to reveal a clear icosahedral-like configuration in the amorphous Zr77Rh23 alloy. It is noteworthy that the splitting in the second peak of the partial PDF implies the existence of a medium range order (MRO) in the Zr77Rh23 system. We obtain the local order in three-dimensional atomic density distributions by using a new atomistic cluster alignment (ACA) method. Interestingly, a Bergman-type MRO is observed in the glassy Zr77Rh23. Furthermore, the spatial distribution and connections of icosahedral-like clusters are shown to further demonstrate the MRO network. Our findings shed light on the nature of atomic local structures of amorphous Zr77Rh23 alloy and have important implications to understanding the formation of various MROs in metallic glasses.

Guo, Y. R.↗
DOE OSTI2017

Sensitivity analysis on chaotic dynamical systems by Non-Intrusive Least Squares Shadowing (NILSS)

This paper develops the Non-Intrusive Least Squares Shadowing (NILSS) method, which computes the sensitivity for long-time averaged objectives in chaotic dynamical systems. In NILSS, we represent a tangent solution by a linear combination of one inhomogeneous tangent solution and several homogeneous tangent solutions. Next, we solve a least squares problem using this representation; thus, the resulting solution can be used for computing sensitivities. NILSS is easy to implement with existing solvers. In addition, for chaotic systems with many degrees of freedom but few unstable modes, NILSS has a low computational cost. NILSS is applied to two chaotic PDE systems: the Lorenz 63 system and a CFD simulation of flow over a backward-facing step. In both cases, the sensitivities computed by NILSS reflect the trends in the long-time averaged objectives of dynamical systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

A dynamic likelihood approach to filtering transport processes: advection-diffusion dynamics

A Bayesian data assimilation scheme is formulated for advection-dominated advective and diffusive evolutionary problems, based upon the Dynamic Likelihood (DLF) approach to filtering. The DLF was developed specifically for hyperbolic problems –waves–, and in this paper, it is extended via a split step formulation, to handle advection-diffusion problems. In the dynamic likelihood approach, observations and their statistics are used to propagate probabilities along characteristics, evolving the likelihood in time. The estimate posterior thus inherits phase information. For advection-diffusion the advective part of the time evolution is handled on the basis of observations alone, while the diffusive part is informed through the model as well as observations. We expect, and indeed show here, that in advection-dominated problems, the DLF approach produces better estimates than other assimilation approaches, particularly when the observations are sparse and have low uncertainty. The added computational expense of the method is cubic in the total number of observations over time, which is on the same order of magnitude as a standard Kalman filter and can be mitigated by bounding the number of forward propagated observations, discarding the least informative data.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2019

Monte Carlo Simulation of Borosilicate Glass Dissolution using Molecular Dynamics-Generated Glass Structures

Atomic-scale insights into the dissolution mechanisms of borosilicate glasses are critical to the development of the waste form corrosion models that inform performance assessments of nuclear waste disposal facilities. Monte Carlo (MC) simulations have been instrumental in advancing the state of knowledge of borosilicate glass dissolution; however, all such simulations to date have relied on lattices to represent the amorphous glass structure, thereby potentially introducing artifacts. Therefore, a new approach, referred to as the amorphous MC approach, has been developed whereby glass structures generated from molecular dynamics simulations are used as starting points for MC simulations of glass dissolution. MC simulations of sodium borosilicate glasses that covered a wide compositional range were performed and revealed correlations between dissolution rate and structural features of the glasses. Notably, the lattice MC approach predicted the fraction of tetrahedral boron to have a lesser influence on the dissolution rate than computed with the amorphous MC approach. The lattice MC simulations also overestimated the dissolution rate for a given glass composition. These findings highlight the importance of using truly amorphous structures in MC simulations of glass corrosion.

Kerisit, Sebastien N.↗
DOE OSTI2023

Atomic Diffusion, Segregation, and Grain Boundary Migration in Nickel-Based Alloys from Molecular Dynamics Simulations

Grain boundary diffusion and metal mobility in alloys control material performance in many applications and yet remain poorly understood at a mechanistic level. With advances in accessible time and length scales for computational molecular simulations, and recent force field developments, we now possess tools to help unravel those mechanisms. Using large-scale molecular dynamics simulations, here we examined vacancy-mediated diffusion processes in Ni-5Cr alloy with low and high-energy grain boundaries. We show that atomic diffusion inside the grain boundary plane is about four times higher than bulk diffusion, at any temperature, and exhibits a typical Arrhenius behavior with a very small energy barrier (0~.8 eV for Cr and 0.7 eV for Ni within 1300-1600 K). Additionally, the fastest diffusing species inverts; Cr diffusion was faster than Ni in the bulk but slower in the grain boundaries. This is attributed to the creation of high cohesive energy clusters of Cr at the grain boundary. Grain boundary migration was also observed to be temperature dependent and appears to be two times higher in the 5% Cr alloy than in pure Ni, highlighting the important role of the alloying element on grain boundary motion.

Simonnin, Pauline GN↗
DOE OSTI2018

Modeling error PDF optimization based wavelet neural network modeling of dynamic system and its application in blast furnace ironmaking

In general, the modeling errors of dynamic system model are a set of random variables. The traditional performance index of modeling such as means square error (MSE) and root means square error (RMSE) can not fully express the connotation of modeling errors with stochastic characteristics both in the dimension of time domain and space domain. Therefore, the probability density function (PDF) is introduced to completely describe the modeling errors in both time scales and space scales. Based on it, a novel wavelet neural network (WNN) modeling method is proposed by minimizing the two-dimensional (2D) PDF shaping of modeling errors. First, the modeling error PDF by the tradional WNN is estimated using data-driven kernel density estimation (KDE) technique. Then, the quadratic sum of 2D deviation between the modeling error PDF and the target PDF is utilized as performance index to optimize the WNN model parameters by gradient descent method. Since the WNN has strong nonlinear approximation and adaptive capability, and all the parameters are well optimized by the proposed method, the developed WNN model can make the modeling error PDF track the target PDF, eventually. Simulation example and application in a blast furnace ironmaking process show that the proposed method has a higher modeling precision and better generalization ability compared with the conventional WNN modeling based on MSE criteria. Furthermore, the proposed method has more desirable estimation for modeling error PDF that approximates to a Gaussian distribution whose shape is high and narrow.

Modelling↗
DOE OSTI2025

Dynamical coupled-channel models for hadron dynamics

Dynamical coupled-channel (DCC) approaches parametrize the interactions and dynamics of two and more hadrons and their response to different electroweak probes. The inclusion of unitarity, three-body channels, and other properties from scattering theory allows for a reliable extraction of resonance spectra and their properties from data. Here, we review the formalism and application of the ANL-Osaka, the Juelich-Bonn-Washington, and other DCC approaches in the context of light baryon resonances from meson, (virtual) photon, and neutrino-induced reactions, as well as production reactions, strange baryons, light mesons, heavy meson systems, exotics, and baryon-baryon interactions. Finally, we also provide a connection of the formalism to study finite-volume spectra obtained in Lattice QCD, and review applications involving modern statistical and machine learning tools.

Amplitude analysis↗
DOE OSTI2019

Heterogeneous CPU+GPU-Enabled Simulations for DFTB Molecular Dynamics of Large Chemical and Biological Systems

We introduce a new heterogeneous CPU+GPU-enhanced DFTB approach for the routine and efficient simulation of large chemical and biological systems. Here, compared to homogenous computing with conventional CPUs, heterogeneous computing approaches exhibit substantial performance with only a modest increase in power consumption, both of which are essential to upcoming exascale computing initiatives. We show that DFTB-based molecular dynamics is a natural candidate for heterogeneous computing since the computational bottleneck in these simulations is the diagonalization of the Hamiltonian matrix, which is performed several times during a single molecular dynamics trajectory. To thoroughly test and understand the performance of our heterogeneous CPU+GPU approach, we examine a variety of algorithmic implementations, benchmarks of different hardware configurations, and applications of this methodology on several large chemical and biological systems. Finally, to demonstrate the capability of our implementation, we conclude with a large-scale DFTB MD simulation of explicitly solvated HIV protease (3,974 atoms total) as a proof-of-concept example of an extremely large/complex system which, to the best of our knowledge, is the first time that an entire explicitly-solvated protein has been treated at a quantum-based MD level of detail.

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

Photo-Induced Charge Transfer of Fullerene and Non-Fullerene Conjugated Polymer Blends via Ab Initio Excited-State Dynamics

Organic conjugated polymers (CPs) are promising candidates for organic photovoltaic (OPV) devices due to their unique tunable mechanical and optoelectronic performance. Over the last decade, optoelectronic properties of narrow band gap CPs as a blend with acceptor units are largely optimized, which leads to noticeable progress in OPV technology. However, their power conversion efficiency is still lower than their organic counterparts (i.e., silicon), limiting their practical usage. In this study, we employ ab initio molecular dynamics to explore photo-induced charge transfer (CT) of the diketopyrrolopyrrole-based polymer as a blend with non-fullerene (i.e., ITIC) and fullerene (i.e., PCBM) acceptor units. The results of charge carrier dynamics induced by selected photoexcitation show that hole density redistribution in space is much faster than electron relaxation. We track the relaxation rates of charge carriers over time, where the derivative of the difference between the rate of electron and hole implies the current density at zero voltage. Furthermore, this can be utilized to characterize the CT performance of CPs blended with different acceptor units. Relaxation rate results indicate that CP blend with ITIC promises a better PV performance, illustrating that the current computational approach opens the door to determine bulk heterojunctions’ electronic performance for OPV devices and narrowing down the list of potential donor–acceptor candidates.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

4D-STEM Mapping of Nanocrystal Reaction Dynamics and Heterogeneity in a Graphene Liquid Cell

Chemical reaction kinetics at the nanoscale are intertwined with heterogeneity in structure and composition. However, mapping such heterogeneity in a liquid environment is extremely challenging. Here, in this work, we integrate graphene liquid cell (GLC) transmission electron microscopy and four-dimensional scanning transmission electron microscopy to image the etching dynamics of gold nanorods in the reaction media. Critical to our experiment is the small liquid thickness in a GLC that allows the collection of high-quality electron diffraction patterns at low dose conditions. Machine learning-based data-mining of the diffraction patterns maps the three-dimensional nanocrystal orientation, groups spatial domains of various species in the GLC, and identifies newly generated nanocrystallites during reaction, offering a comprehensive understanding on the reaction mechanism inside a nanoenvironment. This work opens opportunities in probing the interplay of structural properties such as phase and strain with solution-phase reaction dynamics, which is important for applications in catalysis, energy storage, and self-assembly.

four-dimensional scanning transmission electron mi↗
DOE OSTI2021

Insights into Spontaneous Solid Electrolyte Interphase Formation at Magnesium Metal Anode Surface from Ab Initio Molecular Dynamics Simulations

Spontaneous chemical reactivity at multivalent (Mg, Ca, Zn, Al) electrode surfaces is critical to solid electrolyte interphase (SEI) formation, and hence, directly affects the longevity of batteries. Here, we report an investigation of the reactivity of 0.5 M Mg(TFSI)2 in 1,2-dimethoxyethane (DME) solvent at a Mg(0001) surface using ab initio molecular dynamics (AIMD) simulations and detailed Bader charge analysis. Based on the simulations, the initial degradation reactions of the electrolyte strongly depend on the structure of the Mg(TFSI)2 species near the anode surface. At the surface, the dissociation of Mg(TFSI)2 species occurs via cleavage of the N-S bond for the solvent separated ion pair (SSIP) and via cleavage of the C-S bond for the contact ion pair (CIP) configuration. In the case of the CIP, both TFSI anions undergo spontaneous bond dissociation reactions to form atomic O, C, S, F, and N species adsorbed on the surface of the Mg anode. These products indicate that the initial SEI layer formed on the surface of the pristine Mg anode consists of a complex mixture of multiple components such as oxides, carbides, sulfides, fluorides, and nitrides. We believe that the atomic level insights gained from these simulations will lay the groundwork for the rational design of tailored and functional interphases that are critical for the success of multivalent battery technology.

Agarwal, Garvit↗
DOE OSTI2021

Photocarrier Dynamics in MoTe 2 Nanofilms with 2 H and Distorted 1 T Lattice Structures

Molybdenum telluride (MoTe 2 ), an emerging layered two-dimensional (2D) material, possesses excellent phase-changing properties. Previous studies revealed its reversible transition between 2H and 1T' phases with a transition energy as small as 35 meV. Since 1T'-MoTe 2 is metallic, it can serve as an electrical contact for semiconducting 2H-MoTe 2 -based optoelectronic devices. Here, the photocarrier dynamics in MoTe 2 nanofilms synthesized by a one-step method and with coexisting multiple phases are investigated by transient absorption measurements. Both the energy relaxation time and the recombination lifetime of the excitons are shorter in the 1T'-MoTe 2 compared to its 2H phase. Furthermore, these results provide information on the different photocarrier dynamical properties of these two phases, which is important for future 2D optoelectronic and phase-change electronic devices based on MoTe 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2023

Reversible Reactions, Mesh Size, and Segmental Dynamics Control Penetrant Diffusion in Ethylene Vitrimers

The diffusion of two aromatic dyes with nearly identical sizes was measured in ethylene vitrimers with precise linker lengths and borate ester cross-links using fluorescence recovery after photobleaching (FRAP). One dye possessed a reactive hydroxyl group, while the second was inert. The reaction of the hydroxyl group with the network is slow relative to the hopping times of the dye, resulting in a large slowdown by a factor of 50 for a reactive probe molecule. A kinetic model was fit to the fluorescence intensity data to determine rate constants for the reversible reaction of the dye from the network, which confirms the role of slow reaction kinetics. A second network cross-linker was also investigated with a substituted boronic ester showing ∼10,000 times faster exchange kinetics. In this system, the two dyes show the same diffusion coefficient, as the reaction is no longer the rate-limiting step. The role of dense meshes on small and large dyes is also discussed in the context of the existing theories. Finally, these results highlight the potential of dynamic networks to control penetrant transport through synergistic effects of the mesh size, dynamic bond kinetics, and penetrant–network interactions.

confinement↗
DOE OSTI2015

Dynamics of Back Electron Transfer in Dye-Sensitized Solar Cells Featuring 4-tert-Butyl-Pyridine and Atomic-Layer-Deposition Alumina as Surface Modifiers.

A series of dye-sensitized solar cells (DSCs) was constructed with TiO2 nanoparticles and N719 dye. The standard I-3(-)/I- redox shuttle and the Co(1,10-phenanthroline)(3)(3+/2+) shuttle were employed. DSCs were modified with atomic-layered-deposited (ALD) coatings of Al2O3 and/or with the surface-adsorbing additive 4-tert-butyl-pyridine. Current-voltage data were collected to ascertain the influence of each modification upon the back electron transfer (ET) dynamics of the DSCs. The primary effect of the additives alone or in tandem is to increase the open-circuit voltage. A second is to alter the short-circuit current density, J(SC). With dependence on the specifics of the system examined, any of a myriad of dynamics-related effects were observed to come into play, in both favorable (efficiency boosting) and unfavorable (efficiency damaging) ways. These effects include modulation of (a) charge-injection yields, (b) rates of interception of injected electrons by redox shuttles, and (c) rates of recombination of injected electrons with holes on surface-bound dyes. In turn, these influence charge-collection lengths, charge-collection yields, and onset potentials for undesired dark current. The microscopic origins of the effects appear to be related mainly to changes in driving force and/or electronic coupling for underlying component redox reactions. Perhaps surprisingly, only a minor role for modifier-induced shifts in conduction-band-edge energy was found. The combination of DSC-efficiency-relevant effects engendered by the modifiers was found to vary substantially as a function of the chemical identity of the redox shuttle employed. While types of modifiers are effective, a challenge going forward will be to construct systems in ways in which the benefits of organic and inorganic modifiers can be exploited in fully additive, or even synergistic, fashion.

Katz, Michael J.↗