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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

PYSEQM

PYSEQM is a package for performing semi-empirical quantum mechanical (SEQM) simulations on molecular systems utilizing PyTorch. SEQM simulations determine molecular properties (energy, electron density, dipole moment, ect.) by solving an approximate Schrödinger equation for the motions of electrons in a molecule. The use of PyTorch provides three specific advantages. First, it allows the calculations to be offloaded to GPU accelerators, giving an order of magnitude increase in speed. Second, back propagation is used to get atomic forces (derivative of the total energy with respect to atomic position) at the same computational cost as the energy calculation itself. Finally, the use of PyTorch makes for a natural interface to modern machine learning methods, which can be used to adjust the semi-empirical parameters build into SEQM methods. Additionally, PYSEQM implements various other optimizations for performing quantum mechanics based molecular dynamics, including SP2 for rapid GPU based solution of the self-consistent field algorithm, and the extended Lagrangian method for rapid QM-MD.

Nebgen, Benjamin↗
DOE OSTI2022

Deep learning of dynamically responsive chemical Hamiltonians with semiempirical quantum mechanics

Conventional machine-learning (ML) models in computational chemistry learn to directly predict molecular properties using quantum chemistry only for reference data. While these heuristic ML methods show quantum-level accuracy with speeds several orders of magnitude faster than traditional quantum chemistry methods, they suffer from poor extensibility and transferability; i.e., their accuracy degrades on large or new chemical systems. Incorporating quantum chemistry frameworks into the ML models directly solves this problem. Here we take the structure of semiempirical quantum mechanics (SEQM) methods to construct dynamically responsive Hamiltonians. SEQM methods use empirical parameters fitted to experimental properties to construct reduced-order Hamiltonians, facilitating much faster calculations than ab initio methods but with compromised accuracy. By replacing these static parameters with machine-learned dynamic values inferred from the local environment, we greatly improve the accuracy of the SEQM methods. Trained on molecular energies and atomic forces, these dynamically generated Hamiltonian parameters show a strong correlation with atomic hybridization and bonding. Trained with only about 60,000 small organic molecular conformers, the resulting model retains interpretability, extensibility, and transferability when testing on much larger chemical systems and predicting various molecular properties. Overall, this work demonstrates the virtues of incorporating physics-based descriptions with ML to develop models that are simultaneously accurate, transferable, and interpretable.

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

Hypothetical Efficiency of Electrical to Mechanical Energy Transfer during Individual Stochastic Molecular Switching Events

There are now many examples of single molecule rotors, motors and switches in the literature that, when driven by photons, electrons or chemical reactions, exhibit well defined motions. As a step towards using these single molecule devices to perform useful functions one must understand how they interact with their environment and quantify their ability to perform work on it. Using a single molecule rotary switch we examine the transfer of electrical energy, delivered via electron tunneling, to mechanical motion and measure the forces the switch experiences with a non-contact q-plus atomic force microscope. Action spectra reveal that the molecular switch has two stable states and can be excited resonantly between them at a bias of 100 mV via a one-electron inelastic tunneling process which corresponds to an energy input of 16 zepto Joules. Furthermore, while the electrically induced switching events are stochastic and no net work is to done on the cantilever, by measuring the forces between the molecular switch and the AFM cantilever we can derive the maximum hypothetical work the switch could perform during a single switching event which is ~55 meV, equal to 8.9 zepto Joules which translates to a hypothetical efficiency ~55% per individual inelastic tunneling electron induced switching event. When co considering the total electrical energy input this drops to 1x10 -7 % due to elastic tunneling events that dominate the tunneling current. However, this approach constitutes a general method for quantifying and comparing the energy input and output of molecularmechanical devices.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Evidence for In-Plane Electrical Polarization in 3R-β’-In 2 Se 3 Thin Films Grown by Molecular Beam Epitaxy

β-In 2 Se 3 has been identified as a potential ferroelectric. This work describes the growth of β-In 2 Se 3 via molecular beam epitaxy along with a description of its properties, including the search for switchable polarization in 3R-β’-In2Se3. The thin-film morphology, crystal structure, and phase maps of β-In 2 Se 3 on Si(111) and Al 2 O 3 (0001) were evaluated by atomic force microscopy, X-ray diffraction, and Raman spectroscopy as a function of the atomic Se/In flux ratio and growth temperature. Smooth β-In 2 Se 3 thin films were successfully realized on Si(111) at a substrate temperature of 150 °C using a Se/In flux ratio of 5.7, as well as on Al 2 O 3 (0001) at 450 °C using a Se/In flux ratio of 5.5. Scanning transmission electron microscopy (STEM) confirms the 3R polytype of β-In 2 Se 3 in films on both substrates, with a minor disorder associated with the 2H polytype at the interface. Indications of in-plane Se atom displacements characteristic of the 3R-β’-In 2 Se 3 polytype were found by STEM and second harmonic generation analysis in films on Al 2 O 3 (0001), but not in films on Si(111). Furthermore, attempts at electrical polarization switching did not produce compelling evidence for ferroelectricity. Instead, electrical transport measurements demonstrated locally varying anisotropic responses with the applied electric fields along different in-plane directions, with some hysteresis associated with the trapping of charges.

36 MATERIALS SCIENCE↗
DOE OSTI2024

A dynamic Bayesian optimized active recommender system for curiosity-driven partially Human-in-the-loop automated experiments

Optimization of experimental materials synthesis and characterization through active learning methods has been growing over the last decade, with examples ranging from measurements of diffraction on combinatorial alloys at synchrotrons, to searches through chemical space with automated synthesis robots for perovskites. In virtually all cases, the target property of interest for optimization is defined a priori with the ability to shift the trajectory of the optimization based on human-identified findings during the experiment is lacking. Thus, to highlight the best of both human operators and AI-driven experiments, here we present the development of a human–AI collaborated experimental workflow, via a Bayesian optimized active recommender system (BOARS), to shape targets on the fly with human real-time feedback. Here, the human guidance overpowers AI at early iteration when prior knowledge (uncertainty) is minimal (higher), while the AI overpowers the human during later iterations to accelerate the process with the human-assessed goal. We showcase examples of this framework applied to pre-acquired piezoresponse force spectroscopy of a ferroelectric thin film, and in real-time on an atomic force microscope, with human assessment to find symmetric hysteresis loops. It is found that such features appear more affected by subsurface defects than the local domain structure. This work shows the utility of human–AI approaches for curiosity driven exploration of systems across experimental domains.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Tunable Magnetic Coupling in Graphene Nanoribbon Quantum Dots

Abstract Carbon‐based quantum dots (QDs) enable flexible manipulation of electronic behavior at the nanoscale, but controlling their magnetic properties requires atomically precise structural control. While magnetism is observed in organic molecules and graphene nanoribbons (GNRs), GNR precursors enabling bottom‐up fabrication of QDs with various spin ground states have not yet been reported. Here the development of a new GNR precursor that results in magnetic QD structures embedded in semiconducting GNRs is reported. Inserting one such molecule into the GNR backbone and graphitizing it results in a QD region hosting one unpaired electron. QDs composed of two precursor molecules exhibit nonmagnetic, antiferromagnetic, or antiferromagnetic ground states, depending on the structural details that determine the coupling behavior of the spins originating from each molecule. The synthesis of these QDs and the emergence of localized states are demonstrated through high‐resolution atomic force microscopy (HR‐AFM), scanning tunneling microscopy (STM) imaging, and spectroscopy, and the relationship between QD atomic structure and magnetic properties is uncovered. GNR QDs provide a useful platform for controlling the spin‐degree of freedom in carbon‐based nanostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Effects of interlayer confinement and hydration on capacitive charge storage in birnessite

Nanostructured birnessite exhibits high specific capacitance and nearly ideal capacitive behaviour in aqueous electrolytes, rendering it an important electrode material for low-cost, high-power energy storage devices. The mechanism of electrochemical capacitance in birnessite has been described as both Faradaic (involving redox) and non-Faradaic (involving only electrostatic interactions). To clarify the capacitive mechanism, we characterized birnessite’s response to applied potential using ex situ X-ray diffraction, electrochemical quartz crystal microbalance, in situ Raman spectroscopy and operando atomic force microscope dilatometry to provide a holistic understanding of its structural, gravimetric and mechanical responses. These observations are supported by atomic-scale simulations using density functional theory for the cation-intercalated structure of birnessite, ReaxFF reactive force field-based molecular dynamics and ReaxFF-based grand canonical Monte Carlo simulations on the dynamics at the birnessite–water–electrolyte interface. We show that capacitive charge storage in birnessite is governed by interlayer cation intercalation. We conclude that the intercalation appears capacitive due to the presence of nanoconfined interlayer structural water, which mediates the interaction between the intercalated cation and the birnessite host and leads to minimal structural changes.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Atomic-scale homogeneous plastic flow beyond near-theoretical yield stress in a metallic glass

Abstract The onset of yielding and the related atomic-scale plastic flow behavior of bulk metallic glasses at room temperature have not been fully understood due to the difficulty in performing the atomic-scale plastic deformation experiments needed to gain direct insight into the underlying fundamental deformation mechanisms. Here we overcome these limitations by combining a unique sample preparation method with atomic force microscopy-based indentation, which allows study of the yield stress, onset of yielding, and atomic-scale plastic flow of a platinum-based bulk metallic glass in volumes containing as little as approximately 1000 atoms. Yield stresses markedly higher than in conventional nanoindentation testing were observed, surpassing predictions from current models that relate yield stress to tested volumes; subsequent flow was then established to be homogeneous without exhibiting collective shear localization or loading rate dependence. Overall, variations in glass properties due to fluctuations of free volume are found to be much smaller than previously suggested.

Yu, Jiaxin↗
DOE OSTI2022

Phonons of metallic hydrogen with quantum Monte Carlo

Here, we describe a simple scheme to perform phonon calculations with quantum Monte Carlo (QMC) methods and demonstrate it on metallic hydrogen. Because of the energy and length scales of metallic hydrogen and the statistical noise inherent to QMC methods, the conventional manner of calculating force constants is prohibitively expensive. We show that our alternate approach is nearly 100 times more efficient in resolving the force constants needed to calculate the phonon spectrum in the harmonic approximation. This requires only the calculation of atomic forces, as in the conventional approach, and otherwise little or no programmatic modification.

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

Epitaxial Stabilization of Single-Crystal Multiferroic YCrO 3 Thin Films

We report on the growth of stoichiometric, single-crystal YCrO 3 epitaxial thin films on (001) SrTiO 3 substrates using pulsed laser deposition. X-ray diffraction and atomic force microscopy reveal that the films grew in a layer-by-layer fashion with excellent crystallinity and atomically smooth surfaces. Magnetization measurements demonstrate that the material is ferromagnetic below 144 K. The temperature dependence of dielectric permittivity shows a characteristic relaxor-ferroelectric behavior at T C = 375–408 K. A dielectric anomaly at the magnetic transition temperature indicates a close correlation between magnetic and electric order parameters in these multiferroic YCrO 3 films. These findings provide guidance to synthesize rare-earth, chromite-based multifunctional heterostructures and build a foundation for future studies on the understanding of magnetoelectric effects in similar material systems.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Unveiling the mechanism of surface corrugation formation on a quasi free-standing bi-layer graphene via experimental and modeling investigations

Extensive studies have been conducted to accomplish the controls over the formation of surface corrugations on chemical vapor deposited (CVD) graphene. However, the underlying mechanism of the surface corrugation formation on graphene remains elusive, due to the difficulty delineating the growth-induced surface corrugations from wrinkles formed during graphene transfer with the use of a supporting layer casted on top of the sample. Here, in this study, “quasi free-standing” graphene was realized using the weakly-interacting h-BN layer during a wet transfer process to study the surface corrugation formation on graphene. The weak interaction of graphene with the supporting h-BN layer allows for the growth-induced surface corrugations to be released, enabling the investigation of the primary mechanism for the graphene corrugation behavior during the transfer process. The experimental measurements of surface corrugations were conducted using atomic force microscopy (AFM) to reveal that surface corrugations are formed following the graphene’s crystallographic directions. Density functional theory calculations using the projector augmented-wave (PAW) method and Perdew-Burke-Ernzerhof (PBE) exchange correlation functional were also conducted for two models of “atomic-scale ripples” and “nanoscale wrinkles” and showed that all of them are formed along the crystallographic axis of graphene, which is in good agreement with the experimental observations.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Optimizing Magnetic Force Microscopy Resolution and Sensitivity to Visualize Nanoscale Magnetic Domains

Magnetic force microscopy (MFM) enables mapping local magnetic fields across a sample surface with nanoscale resolution. To perform MFM, an atomic force microscopy (AFM) probe whose tip has been magnetized vertically (i.e., perpendicular to the probe cantilever) is oscillated at a fixed height above the sample surface. The resultant shifts in the oscillation phase or frequency, which are proportional to the magnitude and sign of the vertical magnetic force gradient at each pixel location, are then tracked and mapped. Although the spatial resolution and sensitivity of the technique increases with decreasing lift height above the surface, this seemingly straightforward path to improved MFM images is complicated by considerations such as minimizing topographical artifacts due to shorter range van der Waals forces, increasing the oscillation amplitude to further improve sensitivity, and the presence of surface contaminants (in particular water due to humidity under ambient conditions). In addition, due to the orientation of the probe's magnetic dipole moment, MFM is intrinsically more sensitive to samples with an out-of-plane magnetization vector. Here, high-resolution topographical and magnetic phase images of single and bicomponent nanomagnet artificial spin-ice (ASI) arrays obtained in an inert (argon) atmosphere glovebox with <0.1 ppm O 2 and H 2 O are reported. Further, optimization of lift height and drive amplitude for high resolution and sensitivity while simultaneously avoiding the introduction of topographical artifacts is discussed, and detection of the stray magnetic fields emanating from either end of the nanoscale bar magnets (~250 nm long and <100 nm wide) aligned in the plane of the ASI sample surface is shown. Likewise, using the example of a Ni-Mn-Ga magnetic shape memory alloy (MSMA), MFM is demonstrated in an inert atmosphere with magnetic phase sensitivity capable of resolving a series of adjacent magnetic domains each ~200 nm wide.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Epitaxial columnar growth of strain-free antiferromagnetic Weyl semimetal Mn 3 Sn on wurtzite c -plane GaN/Al 2 O 3 (0001)

Weyl semimetal thin films with excellent crystalline quality are of great interest for antiferromagnetic spintronics. Mn 3 Sn is one Weyl semimetal with great properties and promise for exciting science and applications. It has proven very challenging, however, to grow Mn 3 Sn thin films with smooth surfaces, negligible strain, and excellent crystallinity. In this work, we discuss the successful preparation of epitaxial Mn 3 Sn (0001)-oriented thin films via molecular beam epitaxial growth on c -plane wurtzite GaN which was grown by MBE on Al 2 O 3 (0001). We present the reflection high energy electron diffraction analysis along with x-ray diffraction in order to demonstrate the crystalline quality of the film, and we give atomic models to explain the epitaxial orientation relationships between the crystal lattices of the substrate, GaN layer, and Mn 3 Sn layer. Importantly, we discuss the film lattice parameters as compared to expected values, demonstrating negligible strain both in-plane and out-of-plane . Atomic force microscopy reveals an epitaxial columnar growth mode characterized by flat-top-mesa islands, while scanning tunneling microscopy shows the atomically smooth surfaces of the mesa-top structures. Finally, Rutherford backscattering informs the stoichiometry of the film as well as the layer thicknesses.

Chiral antiferromagnetic material↗
DOE OSTI2021

Visualizing Solution Structure at Solid-Liquid Interfaces using Three-Dimensional Fast Force Mapping

Amongst the challenges for a variety of research fields are the visualization of solid-liquid interfaces and understanding how they are affected by the solution conditions such as ion concentrations, pH, ligands, and trace additives, as well as the underlying crystallography and chemistry. Here, in this context, three-dimensional fast force mapping (3D FFM) has emerged as a promising tool for investigating solution structure at interfaces. This capability is based on atomic force microscopy (AFM) and allows the direct visualization of interfacial regions in three spatial dimensions with sub-nanometer resolution. Here we provide a detailed description of the experimental protocol for acquiring 3D FFM data. The main considerations for optimizing the operating parameters depending on the sample and application are discussed. Moreover, the basic methods for data processing and analysis are discussed, including the transformation of the measured instrument observables into tip-sample force maps that can be linked to the local solution structure. Finally, we shed light on some of the outstanding questions related to 3D FFM data interpretation and how this technique can become a central tool in the repertoire of surface science.

Nakouzi, Elias↗
DOE OSTI2023

Discovery and construction of surface kagome electronic states induced by p-d electronic hybridization in Co3Sn2S2

Abstract Kagome-lattice materials possess attractive properties for quantum computing applications, but their synthesis remains challenging. Herein, based on the compelling identification of the two cleavable surfaces of Co 3 Sn 2 S 2 , we show surface kagome electronic states (SKESs) on a Sn-terminated triangular Co 3 Sn 2 S 2 surface. Such SKESs are imprinted by vertical p-d electronic hybridization between the surface Sn (subsurface S) atoms and the buried Co kagome-lattice network in the Co 3 Sn layer under the surface. Owing to the subsequent lateral hybridization of the Sn and S atoms in a corner-sharing manner, the kagome symmetry and topological electronic properties of the Co 3 Sn layer is proximate to the Sn surface. The SKESs and both hybridizations were verified via qPlus non-contact atomic force microscopy (nc-AFM) and density functional theory calculations. The construction of SKESs with tunable properties can be achieved by the atomic substitution of surface Sn (subsurface S) with other group III-V elements (Se or Te), which was demonstrated theoretically. This work exhibits the powerful capacity of nc-AFM in characterizing localized topological states and reveals the strategy for synthesis of large-area transition-metal-based kagome-lattice materials using conventional surface deposition techniques.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Tunable room-temperature ferromagnetism in Co-doped two-dimensional van der Waals ZnO

The recent discovery of ferromagnetism in two-dimensional van der Waals crystals has provoked a surge of interest in the exploration of fundamental spin interaction in reduced dimensions. However, existing material candidates have several limitations, notably lacking intrinsic room-temperature ferromagnetic order and air stability. Here, motivated by the anomalously high Curie temperature observed in bulk diluted magnetic oxides, we demonstrate room-temperature ferromagnetism in Co-doped graphene-like Zinc Oxide, a chemically stable layered material in air, down to single atom thickness. Through the magneto-optic Kerr effect, superconducting quantum interference device and X-ray magnetic circular dichroism measurements, we observe clear evidences of spontaneous magnetization in such exotic material systems at room temperature and above. Transmission electron microscopy and atomic force microscopy results explicitly exclude the existence of metallic Co or cobalt oxides clusters. X-ray characterizations reveal that the substitutional Co atoms form Co 2+ states in the graphitic lattice of ZnO. By varying the Co doping level, we observe transitions between paramagnetic, ferromagnetic and less ordered phases due to the interplay between impurity-band-exchange and super-exchange interactions. Our discovery opens another path to 2D ferromagnetism at room temperature with the advantage of exceptional tunability and robustness.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ab initio and force field molecular dynamics study of bulk organophosphorus and organochlorine liquid structures

Here, we performed ab initio molecular dynamics (AIMD) simulations to benchmark bulk liquid structures and to evaluate results from all-atom force field molecular dynamics (FFMD) simulations with the generalized Amber force field (GAFF) for organophosphorus (OP) and organochlorine (OC) compounds. Our work also addresses the current and important topic of force field validation, applied here to a set of nonaqueous organic liquids. Our approach differs from standard treatments, which validate force fields based on thermodynamic data. Utilizing radial distribution functions (RDFs), our results show that GAFF reproduces the AIMD-predicted asymmetric liquid structures moderately well for OP compounds that contain bulky alkyl groups. Among the OCs, RDFs obtained from FFMD overlap well with AIMD results, with some offsets in position and peak structuring. However, re-parameterization of GAFF for some OCs is needed to reproduce fully the liquid structures predicted by AIMD. The offsets between AIMD and FFMD peak positions suggest inconsistencies in the developed force fields, but, in general, GAFF is able to capture short-ranged and long-ranged interactions of OPs and OCs observed in AIMD. Along with the local coordination structure, we also compared enthalpies of vaporization. Overall, calculated bulk properties from FFMD compared reasonably well with experimental values, suggesting that small improvements within the FF should focus on parameters that adjust the bulk liquid structures of these compounds.

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

Simple and efficient algorithms for training machine learning potentials to force data

Machine learning models, trained on data from ab initio quantum simulations, are yielding molecular dynamics potentials with unprecedented accuracy. One limiting factor is the quantity of available training data, which can be expensive to obtain. A quantum simulation often provides all atomic forces, in addition to the total energy of the system. These forces provide much more information than the energy alone. It may appear that training a model to this large quantity of force data would introduce significant computational costs. Actually, training to all available force data should only be a few times more expensive than training to energies alone. Here, we present a new algorithm for efficient force training, and benchmark its accuracy by training to forces from real-world datasets for organic chemistry and bulk aluminum.

74 ATOMIC AND MOLECULAR PHYSICS↗