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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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Data Generation for Machine Learning Interatomic Potentials and Beyond

The field of data-driven chemistry is undergoing an evolution, driven by innovations in machine learning models for predicting molecular properties and behavior. Recent strides in ML-based interatomic potentials have paved the way for accurate modeling of diverse chemical and structural properties at the atomic level. The key determinant defining MLIP reliability remains the quality of the training data. A paramount challenge lies in constructing training sets that capture specific domains in the vast chemical and structural space. This Review navigates the intricate landscape of essential components and integrity of training data that ensure the extensibility and transferability of the resulting models. We delve into the details of active learning, discussing its various facets and implementations. We outline different types of uncertainty quantification applied to atomistic data acquisition and the correlations between estimated uncertainty and true error. The role of atomistic data samplers in generating diverse and informative structures is highlighted. Furthermore, we discuss data acquisition via modified and surrogate potential energy surfaces as an innovative approach to diversify training data. The Review also provides a list of publicly available data sets that cover essential domains of chemical space.

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

Inelastic Neutron Scattering from Thin Film Biaxially Oriented Polyethylene Terephthalate

Recent interest in emerging processes for polymer manufacturing and bio-based chemistries for direct chemical recycling/upcycling has motivated new research focused on a deeper understanding of atomic-scale polymer properties and how they influence macroscopic phenomena. Uncovering the fundamental properties of polymers that give rise to macroscopic behavior could enable new pathways for improved recyclability or utilization of alternative “greener” polymer analogues. In this study, the neutron vibrational spectrum was measured for a film of biaxially oriented polyethylene terephthalate (BoPET) using inelastic neutron scattering (INS), to investigate the relationship between the structure and dynamics of a widely used polymer. Compared to conventional spectroscopic techniques, the use of INS is advantageous for polymeric materials due to the absence of selection rules (i.e., all transitions are allowed), broad-band energy range, and considerable sensitivity to hydrogen modes. In order to distinguish the vibrational modes caused by trans and gauche rotational isomerism, the normal modes of vibration were calculated from a density functional theory-optimized structure of crystalline PET (cPET), representative of the all-trans state, and compared with INS from “highly crystalline” PET powder. Although in- and out-of-plane wagging of hydrogens on the ring structure exhibit significant contribution to both BoPET and cPET spectra, the wagging, rocking, and twisting modes of hydrogen on the ethylene glycol group are, in most cases, conformation-specific. These results were further rationalized by investigating the role of hyperconjugation in stabilizing both conformations using the natural bond order method. Here, through comparison of experimental and calculated INS results, this work provides the fundamental basis for discovering the role of structure and dynamics in shaping the macroscopic properties of PET and polymer analogues.

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

A Theoretical Benchmark of the Geometric and Optical Properties for 3d Transition Metal Nanoclusters via Density Functional Theory

Understanding structure–property relationships in atomically precise metal nanoclusters is vital in finding selective and tunable catalysts. Here, in this study, density functional theory (DFT) was used to benchmark seven exchange correlation functionals at different basis sets for 17 atomically precise nanoclusters against experimentally determined geometries, band gaps, and optical gaps. The set contains both monometallic and bimetallic clusters that possess at least two types of 3d transition metals (specifically, Cu, Ni, Fe, or Co). The benchmark highlights that PBE0 is a good functional to use regardless of the basis set, and Minnesota functionals do well with respect to specific metals. Further, while long-range corrected functionals overestimate band and optical gaps, they model absorption features better than the other considered functionals. The study additionally looks at the photoinduced hydrogen evolution reaction (HER) and the CO 2 reduction mechanism on nanoclusters reported from the literature.

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

The Surface Chemistry of Methanol on Cu 3 Pd(111): Effects of Metal Alloying and Reaction with Hydrogen

Synchrotron-based ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) was used to study the adsorption and surface chemistry of methanol on a Cu 3 Pd(111) model surface. The composition and morphological properties of the pristine Cu 3 Pd(111) substrate were analyzed using a combination of low-energy electron diffraction (LEED), scanning tunneling microscopy (STM), and low-energy ion scattering (LEIS). The results of ion scattering showed segregation of Pd toward the surface, with a Pd/Cu ratio close to 0.5, a larger value than the ratio of 0.33 expected for a Cu 3 Pd bimetallic structure. The surface of the alloy exhibited a good LEED pattern with three-fold long-range periodicities. In STM, clusters of palladium with hexagonal arrays and Pd- Pd distances of 2.7-2.8 Å were detected. Bonding to copper perturbed the electronic properties of the atoms in the Pd clusters, shifting their 4d states toward higher binding energy with respect to the Fermi level. Further, the valence band spectrum of Cu 3 Pd(111) exhibited a line shape that was very different from those displayed by Cu(111) or Pd(111). At low pressures, the adsorption of methanol on Cu 3 Pd(111) at 300 K mainly produced CH 3 O, CO and CH x species. AP-XPS showed that most Pd atoms in the surface of the Cu 3 Pd(111) alloy interacted with the decomposition products of methanol. No significant changes were observed in the core levels of copper upon the adsorption and dissociation of methanol, suggesting that the molecule mainly interacted with Pd sites of the alloy. Reaction with hydrogen led to fast removal of CH x , C and PdC x species from Cu 3 Pd(111) at moderate (< 450 K) temperatures and prevented a CH x → C transformation. If the stability of adsorbed CH 3 O is used as a descriptor for the hydrogenation of CO 2 to methanol, Cu 3 Pd should be a much better catalyst than monometallic palladium. This may be a consequence of electronic and ensemble effects in the alloy that moderate the reactivity of Pd sites.

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

Te/CdTe and Al/CdTe Interfacial Energy Band Alignment by Atomistic Modeling

A synergistic approach that incorporates first-principles atomistic modeling with numerical device simulations is used to systematically evaluate the role of heterointerfaces within metal-chalcogenide-based photovoltaic technologies. Two interfaces involving either a tellurium back contact or aluminum back electrode combined with a cadmium telluride absorber layer within cadmium-telluride-based thin-film solar cells are investigated on an atomic scale to determine the mechanisms contributing to variations in device performance. Electronic structures and predicted charge transport behavior with respect to cadmium and tellurium termination of the absorber layer are studied along the polar oriented CdTe{111} facets. The computational methodology reveals a noticeable contrast between the Schottky barrier forming Al/CdTe interface versus the Type I Te/CdTe heterojunction. Greater band bending features are exhibited by the cadmium termination as opposed to the tellurium termination for each interface case. Subsequent device modeling suggests that 3.6% higher photovoltaic conversion efficiency is achievable for the cadmium termination relative to the tellurium termination of the Te/CdTe interface. Based strictly on an idealistic representation, both interface models show the importance of atomic-scale interfacial properties for cadmium telluride solar cell device performance with their bulk properties being validated in comparison to published experimental data. Here, the synergistic approach offers a suitable method to analyze solar cell interfaces through a predictive computational framework for the engineering and optimization of metal-chalcogenide-based thin-film photovoltaic technologies.

Green’s function↗
DOE OSTI2026

Synthetic Tuning of Exciton–Phonon Coupling in Janus WS 2(1-x) Se 2x Monolayers Revealed by Resonant Raman Excitation Spectroscopy for Optoelectronic Applications

Janus monolayers, such as WSSe, have broken out-of-plane symmetry and an intrinsic dipole moment, impacting exciton transport, lifetime, and phonon interactions while imbuing piezoelectric, photocatalytic, and Rashba spin-splitting properties to transition metal dichalcogenides (TMDs). The new properties of this atomically thin material can be used for optoelectronic device applications. As TMDs are converted into Janus monolayers, e.g., top selenization of WS2 to WSSe, the bandgap and structure smoothly evolve, impacting not only the formation of excitons but also their complex interactions with different phonon modes. Resonant Raman excitation profiles (REPs) are uniquely well-suited to reveal both excitonic transitions and exciton–phonon coupling. Here, the resonant REPs of $A^{'}_{1}$ WS 2 and A 1 WSSe modes are measured to understand the strength of their coupling with the A, B, and C excitonic bands of a WS2 monolayer throughout its stepwise transformation into Janus WSSe by pulsed laser deposition (PLD) of energetic selenium species. In situ Raman spectroscopy during deposition is used to controllably prepare stable intermediate Janus structures, WS 2(1-x) Se 2x (0 ≤ x ≤ 0.5), for ex situ measurement of their resonant REPs. As x increases, REPs reveal not only pronounced excitonic bands that gradually shift toward lower photon energies but also strong, mode-selective exciton–phonon coupling. First-principles resonant Raman simulations independently predict this spectral behavior and are shown capable of matching the spectrally broadened, experimentally observed REP profiles in this model system, indicating their strong predictive capability for future experiments. The combination of controlled synthesis, REP characterization, and predictive theory employed here demonstrates a powerful pathway to understand and ultimately tune exciton–phonon interactions for future quantum optical devices.

Janus monolayers↗
DOE OSTI2022

Ab initio predictions link the neutron skin of 208 Pb to nuclear forces

Heavy atomic nuclei have an excess of neutrons over protons, which leads to the formation of a neutron skin whose thickness is sensitive to details of the nuclear force. This links atomic nuclei to properties of neutron stars, thereby relating objects that differ in size by orders of magnitude. The nucleus 208 Pb is of particular interest because it exhibits a simple structure and is experimentally accessible. However, computing such a heavy nucleus has been out of reach for ab initio theory. By combining advances in quantum many-body methods, statistical tools and emulator technology, we make quantitative predictions for the properties of 208 Pb starting from nuclear forces that are consistent with symmetries of low-energy quantum chromodynamics. We explore 10 9 different nuclear force parameterizations via history matching, confront them with data in select light nuclei and arrive at an importance-weighted ensemble of interactions. We accurately reproduce bulk properties of 208 Pb and determine the neutron skin thickness, which is smaller and more precise than a recent extraction from parity-violating electron scattering but in agreement with other experimental probes. This work demonstrates how realistic two- and three-nucleon forces act in a heavy nucleus and allows us to make quantitative predictions across the nuclear landscape.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Machine learning with persistent homology and chemical word embeddings improves prediction accuracy and interpretability in metal-organic frameworks

Machine learning has emerged as a powerful approach in materials discovery. Its major challenge is selecting features that create interpretable representations of materials, useful across multiple prediction tasks. We introduce an end-to-end machine learning model that automatically generates descriptors that capture a complex representation of a material’s structure and chemistry. This approach builds on computational topology techniques (namely, persistent homology) and word embeddings from natural language processing. It automatically encapsulates geometric and chemical information directly from the material system. We demonstrate our approach on multiple nanoporous metal–organic framework datasets by predicting methane and carbon dioxide adsorption across different conditions. Our results show considerable improvement in both accuracy and transferability across targets compared to models constructed from the commonly-used, manually-curated features, consistently achieving an average 25–30% decrease in root-mean-squared-deviation and an average increase of 40–50% in R 2 scores. A key advantage of our approach is interpretability: Our model identifies the pores that correlate best to adsorption at different pressures, which contributes to understanding atomic-level structure–property relationships for materials design.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2021

Quantum Chemistry Common Driver and Databases (QCDB) and Quantum Chemistry Engine (QCEngine): Automation and interoperability among computational chemistry programs

We report that community efforts in the computational molecular sciences (CMS) are evolving toward modular, open, and interoperable interfaces that work with existing community codes to provide more functionality and composability than could be achieved with a single program. The Quantum Chemistry Common Driver and Databases (QCDB) project provides such capability through an application programming interface (API) that facilitates interoperability across multiple quantum chemistry software packages. In tandem with the Molecular Sciences Software Institute and their Quantum Chemistry Archive ecosystem, the unique functionalities of several CMS programs are integrated, including CFOUR, GAMESS, NWChem, OpenMM, Psi4, Qcore, TeraChem, and Turbomole, to provide common computational functions, i.e., energy, gradient, and Hessian computations as well as molecular properties such as atomic charges and vibrational frequency analysis. Both standard users and power users benefit from adopting these APIs as they lower the language barrier of input styles and enable a standard layout of variables and data. These designs allow end-to-end interoperable programming of complex computations and provide best practices options by default.

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

Artificial intelligence for advanced functional materials: exploring current and future directions

This perspective addresses the topic of harnessing the tools of artificial intelligence (AI) for boosting innovation in functional materials design and engineering as well as discovering new materials for targeted applications in energy storage, biomedicine, composites, nanoelectronics or quantum technologies. It gives a current view of experts in the field, insisting on challenges and opportunities provided by the development of large materials databases, novel schemes for implementing AI into materials production and characterization as well as progress in the quest of simulating physical and chemical properties of realistic atomic models reaching the trillion atoms scale and with near ab initio accuracy.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ab Initio Nuclear Thermodynamics

Here, we propose a new Monte Carlo method called the pinhole trace algorithm for ab initio calculations of the thermodynamics of nuclear systems. For typical simulations of interest, the computational speedup relative to conventional grand-canonical ensemble calculations can be as large as a factor of one thousand. Using a leading-order effective interaction that reproduces the properties of many atomic nuclei and neutron matter to a few percent accuracy, we determine the location of the critical point and the liquid-vapor coexistence line for symmetric nuclear matter with equal numbers of protons and neutrons. We also present the first ab initio study of the density and temperature dependence of nuclear clustering.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Achieving sub-0.5-angstrom–resolution ptychography in an uncorrected electron microscope

Subangstrom resolution has long been limited to aberration-corrected electron microscopy, where it is a powerful tool for understanding the atomic structure and properties of matter. Here, we demonstrate electron ptychography in an uncorrected scanning transmission electron microscope (STEM) with deep subangstrom spatial resolution down to 0.44 angstroms, exceeding the conventional resolution of aberration-corrected tools and rivaling their highest ptychographic resolutions​. Our approach, which we demonstrate on twisted two-dimensional materials in a widely available commercial microscope, far surpasses prior ptychographic resolutions (1 to 5 angstroms) of uncorrected STEMs. We further show how geometric aberrations can create optimized, structured beams for dose-efficient electron ptychography. Our results demonstrate that expensive aberration correctors are no longer required for deep subangstrom resolution.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Modulating ion-binding at macromolecular interfaces during (bio)mineralization: A snapshot review for calcium carbonate and calcium phosphate systems

Abstract Local environments have strict influence over (bio)mineralization in calcifying systems. This snapshot review discusses recent insights into the roles of Ca 2+ -macromolecule interactions on the nucleation of calcium carbonate and calcium phosphate minerals. Experimental findings combined with simulations/modeling are providing breakthrough information and raising important questions for future studies. The emerging picture is that both nucleation and growth are driven by local ordering of ions and water about the macromolecule interface, rather than broader properties or molecular class. Tuning macromolecular properties at the atomic scale thus provides opportunities for highly specific controls on mineralization; however, many limitations and challenges remain. We highlight studies employing in-situ atomic force microscopy (AFM) and transmission electron microscopy (TEM) to observe crystallization processes on or near macromolecular substrates. As the distribution and ability of these techniques increases, fundamental studies integrating experimental and computational methods will be crucial to inform a broad range of applications. Graphical abstract

Knight, Brenna M. (ORCID:0000000244000067)↗
DOE OSTI2022

Revealing conductivity of p-type delta layer systems for novel computing applications

This project uses a quantum simulation technique to reveal the true conducting properties of novel atomic precision advanced manufacturing materials. With Moore's law approaching the limit of scaling for the CMOS technology, it is crucial to provide the best computing power and resources to National Security missions. Atomic precision advanced manufacturing-based computing systems can become the key to the design, use, and security of modern weapon systems, critical infrastructure, and communications. We will utilize the state-of-the-art computational methodology to create a predictive simulator for p-type atomic precision advanced manufacturing systems, which may also find applications in counterfeit detection and anti-tamper.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Nuclear Structure Studies at the Limits of Stability

On the quest for a predictive model of atomic nuclei, the properties of rare isotopes have emerged as critical observables that benchmark extrapolations, identify missing physics ingredients in models, or that enable discovery science. Formerly NSCL and now FRIB facilitate world-leading experiments due to the availability of fast, stopped, and reaccelerated rare-isotope beams in conjunction with unique instruments. DOE-SC NP Award DE-SC0020451 supported from 2019 to 2023 MSU’s nuclear structure and reactions program that tackles compelling questions in the field with complementary techniques, probing single-particle and collective degrees of freedom in relevant regions of the nuclear chart and enabled developments that positioned the PIs and their research groups for first FRIB science.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Tunable Few-Layer van der Waals Crystals and Heterostructures as Emerging Energy and Quantum Materials (Final Technical Report)

2D and layered (van der Waals) semiconductors offer extraordinary opportunities for manipulating optically excited charge carriers, many-body excitations, and non-charge based quantum numbers. To date, research has focused on a limited group of materials, mostly transition metal dichalcogenides in the monolayer limit. Other van der Waals semiconductors, and especially few-layer to multilayer crystals and their heterostructures, carry large potential for the discovery of phenomena of interest for future energy and information technologies. But they remain largely unexplored, often due to a lack of access to high-quality materials and approaches for measuring their properties at the relevant scales. The goal of this project was to develop an EPSCoR-State/National Laboratory Partnership that addresses the challenges of preparing high-quality van der Waals semiconductors and of probing their structure, composition, and especially their optoelectronic and photonic properties, near the atomic scale using electron microscopy techniques. A central component of the project was the development of advanced methods for electron microscopy and electron-excited spectroscopy, taking advantage of unique samples as well as leading capabilities and expertise at the partner institutions. Efforts to advance leading-edge techniques was supported by ancillary developments, such as precision sample preparation for electron microscopy/spectroscopy, coordinated chemical imaging, and analytical electron microscopy. Experiments in materials synthesis and technique development were closely linked to theory and computation. The results obtained under this project yielded multifaceted benefits to the involved partners and their institutions, DOE-BES, the wider scientific community, and society at large, particularly in the State of Nebraska through dividends from knowledge and human capital generated under the project.

36 MATERIALS SCIENCE↗