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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 541 records · Page 30
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DOE OSTI2026

Single-Molecule Electron Transport in Peptoids

Peptoids are structural analogs of peptides in which side chains are appended to the backbone nitrogen rather than the α-carbon. The sequence-defined modularity of peptoids enables precise control over structure−function relationships, enabling applications in energy storage and biomedical materials. Despite recent progress, the role of sequence and conformation on electron transport in peptoid molecules is not fully understood. Here, we synthesize a library of peptoid oligomers and characterize their molecular electronic properties using the scanning tunneling microscope-break junction (STM-BJ) technique. Our results show well-defined electron transport behavior for peptoid sequences containing aromatic side groups lacking hydrogen bonds (H-bonds) and without chemical substitutions at the N−C α position. This behavior fundamentally differs from electron transport in peptides, where H-bond interactions give rise to higher conductance states. All-atom molecular dynamics (MD) simulations are used to understand the conformational heterogeneity of peptoids, and molecular conformations obtained from MD simulations are used in quantum mechanical calculations based on the nonequilibrium Green’s function−density functional theory (NEGF-DFT) formalism. In all cases, computational results are in reasonable qualitative agreement with experiments. Our work demonstrates that the conductance behavior of peptoids depends on monomer identity, including side-chain aromaticity and substitution at the N−C α position. Overall, this work provides new insights into the structure−function relationships governing electron transport in peptoid-based materials and establishes design rules for peptoid-based molecular junctions.

Charge transport↗
DOE OSTI2026

Revealing EDL-driven reduction mechanisms in binary, ternary, and quaternary fluorinated electrolytes via an integrated MD–DFT–ML framework

Accurately predicting solid electrolyte interphase (SEI) formation requires explicitly resolving the electric double layer (EDL) structure, which deviates significantly from that of the bulk electrolyte. Although an established molecular dynamics (MD) and Density Functional Theory (DFT) framework can model SEI formation by evaluating reduction reactions of local clusters in the EDL, it suffers from a combinatorial computational bottleneck. To overcome this limitation, we introduce a machine-learning-accelerated simulation workflow (MD–DFT–ML), integrating a gradient-boosted regression model trained on EDL composition data to efficiently predict reduction potentials. We apply this framework to seven fluorinated electrolytes comprising fluorinated anions, a fluorinated ester solvent, two types of diluent (ion-solvating ester vs. non-solvating ether), and an FEC additive. The analysis shows that the EDL selectively accumulates cation-binding species; consequently, the non–cation-binding ether diluent rarely enters the EDL and makes minimal contributions to SEI formation. DFT calculations on statistically representative EDL clusters provide reduction potentials and fluorine-release pathways, while the ML model, which substantially reduces the DFT workload, predicts cluster reduction energies with a mean absolute error of 0.1 eV. The combined MD–DFT–ML approach also quantifies contributions from different sources to LiF formation in the SEI. This methodology establishes a generalizable route for multiscale modeling electrolyte and interphase design for next-generation electrochemical energy-storage systems.

DFT-MD-ML workflow↗
DOE OSTI2025

Barrierless nucleation in glassy precursors drives zeolite formation

Zeolites are crystalline, microporous silicates widely used in catalysis and separations, yet the molecular mechanisms of their formation remain unresolved. Experiments indicate that hydrothermal synthesis of silica zeolites from clear solution proceeds through amorphous nanoaggregates that gradually develop zeolite order in an apparently continuous amorphous to crystal transformation. Here, we combine molecular simulations with advanced algorithms that identify zeolite order and computer vision to elucidate the pathway from clear solution to zeolite nanocrystal. We show that at conditions of hydrothermal synthesis of silica zeolites, the transformation of precursor aggregate into zeolite is not limited by nucleation barriers but by the slow dynamics of reorganization in the glassy precursor matrix. The negligible nucleation barriers result in spinodal-like crystallization that leads to a gradual formation of a mosaic of small crystallites that explain the seemingly continuous character of zeolite crystallization and the catalytic activity of X-ray amorphous, protozeolites and embryonic zeolites. We find that zeolite-like porosity and short-range order emerge early within glassy precursors, well before crystallinity is detected in transmission electron microscopy (TEM) images or X-ray diffraction. The nanoaggregate’s temperature-size phase diagram reveals a convergence of the zeolite–amorphous equilibrium and maximum crystallization rate at ~3 nm diameter nanoparticle diameters and ~200 °C. This convergence signals the termination of the first-order amorphous-to-zeolite transition. Our results provide a unifying framework for understanding nucleation of silica zeolites from solution and suggest that barrierless nucleation may govern the formation of other nanoparticle systems, including minerals and oxides synthesized far below their bulk melting points.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Role of Dynamic Polarization Interactions in the Electrical Double Layer at Calcite (104) Interfaces with Aqueous Solutions

Reactions at mineral interfaces with aqueous solutions control many geochemical and biogeochemical processes in the Earth’s critical zone. At the molecular level, insights into important properties such as the structure of the electrical double layer (EDL) at specific mineral interfaces continue to improve due to the increasing fidelity of laboratory instrumentation and computational approaches. However, molecular simulation approaches suffer from limited reach into relevant scales of time, length, and system complexity. To span this gap, a novel hybrid approach that couples first principle plane-wave density functional theory (DFT) with classical DFT (cDFT) is demonstrated and applied to calcite (104) interfaces with various electrolytes. In this approach, a region of interest described using DFT interacts with the surrounding medium described using cDFT to arrive at a self-consistent ground state. Benchmarking against experimental observations and entirely first principle DFT simulations demonstrates that this hybrid model efficiently encompasses the key short-range and collective interactions in the EDL. Simulations of calcite (104)/solution interfaces reveal the key static and dynamic polarization interactions that give rise to structuring of ions and water. Ion hydration interactions have the strongest effect on the depth of the first minimum in the density distribution of counterions at the surface, and the position and width of the first density peak is largely determined by the strength of ion-correlation forces. Finer details of ion distributions are controlled by mutual polarization of the calcite surface and interfacial electrolyte. Finally, this new ability to efficiently and rigorously predict EDL structure at mineral surfaces in contact with complex solutions paves the way to accurately modeling sorption, nucleation, dissolution, and growth in realistic systems.

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

Assembly and Analysis of Cell-Scale Membrane Envelopes

The march toward exascale computing will enable routine molecular simulation of larger and more complex systems, for example, simulation of entire viral particles, on the scale of approximately billions of atoms-a simulation size commensurate with a small bacterial cell. Anticipating the future hardware capabilities that will enable this type of research and paralleling advances in experimental structural biology, efforts are currently underway to develop software tools, procedures, and workflows for constructing cell-scale structures. Herein, we describe our efforts in developing and implementing an efficient and robust workflow for construction of cell-scale membrane envelopes and embedding membrane proteins into them. A new approach for construction of massive membrane structures that are stable during the simulations is built on implementing a subtractive assembly technique coupled with the development of a structure concatenation tool (fastmerge), which eliminates overlapping elements based on volumetric criteria rather than adding successive molecules to the simulation system. Using this approach, we have constructed two "protocells" consisting of MARTINI coarse-grained beads to represent cellular membranes, one the size of a cellular organelle and another the size of a small bacterial cell. The membrane envelopes constructed here remain whole during the molecular dynamics simulations performed and exhibit water flux only through specific proteins, demonstrating the success of our methodology in creating tight cell-like membrane compartments. Extended simulations of these cell-scale structures highlight the propensity for nonspecific interactions between adjacent membrane proteins leading to the formation of protein microclusters on the cell surface, an insight uniquely enabled by the scale of the simulations. We anticipate that the experiences and best practices presented here will form the basis for the next generation of cell-scale models, which will begin to address the addition of soluble proteins, nucleic acids, and small molecules essential to the function of a cell.

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

Optimized utilization of COMB3 reactive potentials in LAMMPS

An investigation to optimize the application of the third-generation charge optimized many-body (COMB3) interatomic potential and associated input parameters was carried out through the study of solid–liquid interactions in classical molecular dynamics simulations. The rates of these molecular interactions are understood through the wetting rates of water nano-droplets on a bare copper (111) surface. Implementing the Langevin thermostat, the influence of simulation time step, the number of atoms in the system, the frequency at which charge equilibration is performed, and the temperature relaxation rate are all examined. The results indicate that time steps of 0.4 fs are possible when using longer relaxation times for the system temperature, which is almost double the typical time step used for reactive potentials. Additionally, the use of the charge equilibration allows for a fewer atomic layers to be used in the Cu slab. In addition, charge equilibrium schemes do not need to be performed every time step to ensure accurate charge transfer. Interestingly, the rate of wetting for the nanodroplets is dominantly dependent on the temperature relaxation time, which is predicted to significantly change the viscosity of the water droplets. This work provides a pathway for optimizing simulations using the COMB3 reactive interatomic potential.

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

From anti-Arrhenius to Arrhenius behavior in a dislocation-obstacle bypass: Atomistic simulations and theoretical investigation

Dislocations are the primary carriers of plasticity in metallic materials. Understanding the basic mechanisms for dislocation movement is paramount to predicting the material mechanical response. Relying on atomistic simulations, we observe a transition from non-Arrhenius to Arrhenius behavior in the rate of an edge dislocation overcoming the long-range elastic interaction with a prismatic loop in tungsten. Close to the critical resolved shear stress, the process shows a non-Arrhenius behavior at low temperatures. However, as the temperature increases, the activation entropy starts to dominate, leading to a traditional Arrhenius-like behavior. Here, we have computed the activation entropy analytically along the minimum energy path following Schoeck’s method, which captures the cross-over between anti-Arrhenius and Arrhenius domains. Also, the Projected Average Force Integrator (PAFI), another simulation method to compute free energies along an initial transition path, exhibits considerable concurrence with Schoeck’s formalism. We conclude that entropic effects need to be considered to understand processes involving dislocations bypassing elastic barriers close to the critical resolved shear stress. More work needs to be performed to fully understand the discrepancies between Schoeck’s and PAFI compared to molecular dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Computational study of the electrostatic potential and charges of multivalent ionic liquid molecules

The electrostatic interactions in ionic liquids (ILs) can be difficult to quantify, but this information is very valuable for improving intermolecular potentials for performing molecular-level simulations. Although polarizable forcefields can provide improved accuracy, the computational efficiency of fixed charge molecular models is often preferred for larger systems. Here, we propose a multi-scale screening approach for analyzing the charge scaling behavior and other electrostatic properties of ILs, which is more attainable than previous analysis methods that rely on the IL crystalline structures. Based on isolated molecules and small clusters, we study the electrostatic potential properties and charges of multivalent IL molecules using density-functional theory calculations and ab initio molecular dynamics simulations. The charges of the IL molecules are calculated and compared using several different charge estimation techniques. Although there are some differences among the estimated partial charges on the atoms, the total anion and cation charges are very similar. In conclusion, the charge scaling factors are substantial, and they are only slightly affected by the IL cluster size model.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Cyclic Peptides for Lanthanide Binding

Lanthanide ions are difficult to separate from one another due to their similar chemical properties. The discovery of lanthanide-binding peptides and proteins in nature has led to an increased interest in the possibility of utilizing the strong binding of peptides to lanthanide ions for their separations; as such, there has been an effort to identify or design peptides with improved lanthanide binding and selectivity toward particular lanthanide ions. Here, in this study, we designed and characterized lanthanide-binding cyclic peptides (LBCPs) with molecular dynamics simulations, electronic structure calculations, and emission spectroscopy. Luminescent decay measurements were done to determine the number of water molecules coordinated to the Eu 3+ ion in Eu-LBCP complexes and compare to the predicted number of water molecules by computation to assess the lanthanide-binding affinity of LBCPs. Measured stability constants show binding of the LBCPs to the Eu 3+ ion with stronger than micromolar affinity. We were able to identify multiple peptides that selectively bind to middle lanthanides. We describe the structural basis of the lanthanide-binding selectivity trend with strongest binding to the middle lanthanides, followed by the heavier lanthanides, and finally to the lighter ions.

ions↗
DOE OSTI2025

Strain release by 3D atomic misfit in fivefold twinned icosahedral nanoparticles with amorphization and dislocations

Multiple twinning to form fivefold twinned nanoparticles in crystal growth is common and has attracted broad attention ranging from crystallography research to physical chemistry and materials science. Lattice-misfit strain and defects in multiple twinned nanoparticles (MTP) are key to understand and tailor their electronic properties. However, the structural defects and related strain distributions in MTPs are poorly understood in three dimensions (3D). Here, we show the 3D atomic misfit and strain relief mechanism in fivefold twinned icosahedral nanoparticles with amorphization and dislocations by using atomic resolution electron tomography. We discover a two-sided heterogeneity in variety of structural characteristics. A nearly ideal crystallographic fivefold face is always found opposite to a less ordered face, forming Janus-like icosahedral nanoparticles with two distinct hemispheres. The disordered amorphous domains release a large amount of strain. Molecular dynamics simulations further reveal the Janus-like icosahedral nanoparticles are prevalent in the MTPs formed in liquid-solid phase transition. This work provides insights on the atomistic models for the modelling of formation mechanisms of fivefold twinned structures and computational simulations of lattice distortions and defects. We anticipate it will inspire future studies on fundamental problems such as twin boundary migration and kinetics of structures in 3D at atomic level.

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

Influence of misfit dislocations on ionic conductivity at oxide interfaces

Mismatched complex oxide thin films and heterostructures have gained significant traction for use as electrolytes in intermediate temperature solid oxide fuel cells, wherein interfaces exhibit variation in ionic conductivity as compared to the bulk. Although misfit dislocations present at interfaces in these structures impact ionic conductivity, the fundamental mechanisms responsible for this effect are not well understood. To this end, a kinetic lattice Monte Carlo (KLMC) model was developed to trace oxygen vacancy diffusion at misfit dislocations in SrTiO 3 /BaZrO 3 heterostructures and elucidate the atomistic mechanisms governing ionic diffusion at oxide interfaces. The KLMC model utilized oxygen vacancy migration energy barriers computed using molecular statics. While some interfaces promote oxygen vacancy diffusion, others impede their transport. Fundamental factors such as interface layer chemistry, misfit dislocation structure, and starting and ending sites of migrating ions play a crucial role in oxygen diffusivity. Molecular dynamics (MD) simulations were further performed to support qualitative trends for oxygen vacancy diffusion. Overall, the agreement between KLMC and MD is quite good, though MD tends to predict slightly higher conductivities, perhaps a reflection of nuanced structural relaxations that are not captured by KLMC. The current framework comprising KLMC modeling integrated with molecular statics offers a powerful tool to perform mechanistic studies focused on ionic transport in thin film oxide electrolytes and facilitate their rational design.

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

Disentangling cation effects on ion mobility and structure in ionic liquid electrolytes

Ionic liquids (ILs) are low-temperature molten salts, where ion transport is primarily governed by ion–ion interactions. Yet, the impact of organic IL cations on critical electrolyte properties such as ion dissociation and overall transport behavior in lithium-salt-doped ILs remains poorly understood. Moreover, despite their critical role in designing IL-based electrolytes for energy storage applications, ion–ion interactions and ion-specific transport under an applied electrical potential are seldom quantified, largely due to the unique experimental and computational challenges involved. Herein, we compare transport properties obtained using 1 H, 7 Li, and 19 F pulsed-field gradient nuclear magnetic resonance (NMR) and electrophoretic NMR (eNMR) with those measured by electrochemical impedance spectroscopy. Non-equilibrium molecular dynamics (MD) simulations and eNMR confirm the presence of negatively charged [Li(TFSI) n ] (1−n) aggregates that migrate towards the positive electrode, resulting in negative lithium transference numbers. Equilibrium MD simulations reveal a vehicular Li ion transport mechanism facilitated by long-lived aggregates with Li + cations strongly bound to multiple TFSI − anions. Finally, we observe an inverse relationship between the apparent charge of the TFSI − anion in the neat IL, which is dictated by the IL cation, and Li + transport in the salt-doped systems. This highlights the opportunity to tune electrolyte performance by tailoring cation chemistry.

Li-ion batteries↗
DOE OSTI2025

Resolving the Solvation Structure and Transport Properties of Aqueous Zinc Electrolytes from Salt-in-Water to Water-in-Salt Using Neural Network Potential

Zn Cl 2 solutions are promising electrolytes for aqueous zinc-ion batteries. Here, we report a joint computational and experimental study of the structural and dynamic properties of aqueous Zn Cl 2 electrolytes with concentrations ranging from salt-in-water to water-in-salt (WIS). By developing a neural network potential (NNP) model, we perform molecular dynamics (MD) simulations with accuracy but at much larger lengths and longer timescales. The NNP predicted structures are validated by the structure factors measured by X-ray total scattering experiments. The MD trajectories provide a comprehensive and quantitative picture of the Zn 2 + solvation shell structures. Additionally, we find that the O − H covalent bonds in water are strengthened with increasing salt concentration, thus expanding the electrochemical stability window of aqueous electrolytes. In terms of dynamic properties, the calculated and experimentally measured conductivities are in good agreement. Through the analysis of the calculated cation transference number, we propose a three-stage charge carrier transport mechanism with increasing concentration: independent ion transport, strongly correlated ion transport, and small positive charge carrier diffusion through negatively charged polymeric clusters. Our study provides fundamental atomic scale insights into the structure and transport properties of the Zn Cl 2 electrolyte that can aid the optimization and development of WIS electrolytes. Published by the American Physical Society 2025

25 ENERGY STORAGE↗
DOE OSTI2020

Simplified Ab Initio Molecular Dynamics-Based Raman Spectral Simulations

We describe a simplified approach to simulating Raman spectra from ab initio molecular dynamics (AIMD) calculations. The protocol relies on on-the-fly calculations of approximate molecular polarizabilities using the well-known sum over orbitals (as opposed to states) method. This approach bypasses the more accurate but computationally expensive approach to calculating molecular polarizabilities along AIMD trajectories, i.e., solving the coupled perturbed Hartree–Fock/Kohn–Sham equations. We demonstrate the advantages and limitations of our method through a few case studies targeting molecular systems of interest to surface- and/or tip-enhanced Raman spectroscopy practitioners.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

High temperature stability and transport characteristics of hydrogen in alumina via multiscale computation

Here, the impact of hydrogen charge states on the stability and transport characteristics of hydrogen interstitials in alumina polymorphs is evaluated by multiscale computational methods including density functional theory (DFT), ab initio molecular dynamics (AIMD) and machine learned force fields. Thermodynamic calculations show that the protonic H i +1 interstitial is the most stable defect species for most values of the electronic bandgap in both and amorphous alumina (Al 2 O 3 ). Further, active learned Gaussian approximation potentials (GAP) were developed using AIMD data to study temperature dependent long time proton diffusion in alumina. Diffusivity calculations from GAP-MD simulations are found to be comparable with of the AIMD data, while being ~340 times faster and scalable to larger systems. Comparisons with diffusivity values for other interstitial charge states (H i 0 and H i -1 ) and published experimental literature indicate that H i +1 diffusion is the likely mechanism of hydrogen transport. A good agreement is obtained between H i +1 diffusivity calculated in α-Al 2 O 3 from DFT: 5.05 10 -3 exp(-0.81 eV/k B /T) cm 2 /s and reported experiment: 9.7X10 -4 exp(-0.83 eV/k B /T) cm 2 /s. Computationally and experimentally calculated energy barriers (0.81 and 0.83 eV respectively) only differ by 2.5%. Similarly, the pre-exponential diffusion coefficients only differ by 0.5 orders of magnitude. Moreover, the diffusivity of H i +1 in amorphous Al 2 O 3 in the 1000–2000 K range is calculated to be 2.53X10 -2 exp(-0.89 eV/k B /T), just one order of magnitude higher than the corresponding value in α-Al 2 O 3 . This suggests that local structural disorder does not significantly affect the energy landscape and diffusion behavior of H i +1 in Al 2 O 3 . Overall, these results show promise for the application of alumina polymorphs as hydrogen permeation barriers.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Elucidating the Role of Hydrogen at c‐In 2 O 3 /a‐In 2 O 3− x Interface

Ab initio molecular dynamics simulations and hybrid functional electronic structure calculations are employed to determine the formation, the structural and electronic properties, and the dynamics of covalent (In—OH) and ionic (In—H—In) hydrogen defects at crystalline-In 2 O 3 /amorphous-In 2 O 3−x interface. This comprehensive computational study considers (i) various interstitial and substitutional hydrogen site locations within the crystalline, amorphous, and interfacial regions; (ii) several oxygen-to-hydrogen ratios; and (iii) possible defect charged states. The results reveal hydrogen's inability to fully passivate the undercoordinated under-shared in atoms in amorphous highly substoichiometric oxide, giving rise to the formation of deep electron traps even in net-charge neutral structures. These trap defects are found to be sensitive to photoexcitation, in contrast to In—OH with H's electronic states located below the valence band and to In—H—In, where H is found to maintain its charge state upon illumination. Nevertheless, H plays a critical role in photoinduced conductivity and its relaxation by promoting In—O coordination transformations at the interfacial region, including deterioration of the crystalline layer. Finally, the results help identify mobile H species and metastable H defect complexes (such as In—H—H—In, In—OH–H—In, and In—OH–O—In) that are responsible for long relaxation times of the conductivity decay.

H defects↗
DOE OSTI2025

Lattice structure and dynamics of sparse molecular crystals: OsO4 and RuO4

This dataset contains input and output files from DFT simulations used to reproduce the electronic and phonon calculations of bulk and molecular OsO₄ and RuO₄. The files include data from initial electronic structure and phonon calculations performed using different functionals: PBE, PBEsol, and vdW-DF-optB86b. The computed phonon frequencies are compared with Raman crystal and gas-phase frequencies from existing literature, while the calculated phonon density of states (PhDOS) is compared with experimental PhDOS data.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Pressure Effects on the Relaxation of an Excited Ethane Molecule in High-Pressure Bath Gases

Here, we use molecular dynamics to calculate the rotational and vibrational energy relaxation of C 2 H 6 in Ar, Kr, and Xe bath gases over a pressure range of 10 to 400 atm and at temperatures of 300 K and 800 K. The C 2 H 6 is instantaneously excited by 80 kcal/mol randomly distributed into both vibrational and rotational modes. The computed relaxation rates show little sensitivity to the identity of the noble gas in the bath. Vibrational relaxation rates show a non-linear pressure dependence at 300 K. At 800 K the reduced range of bath gas densities covered by the range of pressures do not yet show any non-linearity in the pressure dependence. Rotational relaxation is characterized with two relaxation rates. The slower rate is comparable to the vibrational relaxation rate. The faster rate has a linear pressure dependence at 300 K but an irregular, nonlinear pressure dependence at 800 K. To understand this, a model was developed based on approximating the periodic box used in the molecular dynamics simulations by an equal-volume collection of cubes where each cube is sized to allow only single occupancy by the noble gas or the molecule. Combinatorial statistics then leads to a pressure and temperature dependent analytic distribution of the bath gas species the molecule encounters in a collision. This distribution, the dissociation energy of molecule/bath gas complexes and bath gas clusters, and the computed energy release per collision combine to show that only at 300 K is the energy release sufficient to dissociate likely complexes and clusters. This suggests that persistent and pressure-dependent clusters and complexes at 800 K may be responsible for the non-linear pressure dependence of rotational relaxation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗