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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Existence of La-site antisite defects in LaMO 3 (M = Mn, Fe, and Co) predicted with many-body diffusion quantum Monte Carlo

The properties of LaMO 3 (M: 3d transition metal) perovskite crystals are significantly dependent on point defects, whether introduced accidentally or intentionally. The most studied defects in La-based perovskites are the oxygen vacancies and doping impurities on the La and M sites. Here, we identify that intrinsic antisite defects, the replacement of La by the transition metal, M, can be formed under M-rich and O-poor growth conditions, based on results of an accurate many-body ab initio approach. Our fixed-node diffusion Monte Carlo (FNDMC) calculations of LaMO 3 (M = Mn, Fe, and Co) find that such antisite defects can have low formation energies and are magnetized. Complementary density functional theory (DFT)-based calculations show that Mn antisite defects in LaMnO 3 may cause the p-type electronic conductivity. These features could affect spintronics, redox catalysis, and other broad applications. Our bulk validation studies establish that FNDMC reproduces the antiferromagnetic state of LaMnO 3 , whereas DFT with PBE (Perdew–Burke–Ernzerhof), SCAN (strongly constrained and appropriately normed), and the LDA+U (local density approximation with Coulomb U) functionals all favor ferromagnetic states, at variance with experiment.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Nuclear Theory from First Principles to Forefront Experiments (Final Report for DE-SC0018638)

The Lee research group is a part of the Nuclear Lattice Effective Field Theory Collaboration, which has developed and performed ab initio lattice simulations of nuclear structure, scattering, reactions, and many-body systems. The other senior members of the collaboration include Ulf-G. Meißner at Bonn/Julich, Evgeny Epelbaum and Hermann Krebs at Bochum, Timo Lahde and Thomas Luu at Julich, and Gautam Rupak at Mississippi State. Our letter “Ab initio alpha-alpha scattering” was featured in a Nature News and Views article. Another letter “Nuclear binding near a quantum phase transition” was highlighted in a Viewpoint article in the online APS journal Physics as well as a news article in the IOP publication Physics World (September 21, 2016). Our letter “Eigenvector continuation with subspace learning” was also highlighted a Synopsis article in Physics. There are many promising ab initio approaches being used to calculate the properties of few-and many-nucleon systems. This includes the no-core shell model, symmetry-adapted no-core shell model quantum Monte Carlo, auxiliary-field diffusion Monte Carlo, self-consistent Green’s functions, many-body perturbation theory, in-medium similarity renormalization group, and coupled cluster methods. Lattice effective field theory is another ab initio approach which combines the framework of effective field theory with lattice Monte Carlo methods to allow favorable scaling from few- to many-body systems. Perhaps the most important aspect of lattice effective field theory is that its strengths and weaknesses are orthogonal to that of other ab initio methods. For example, lattice effective field theory has little difficulty in probing cluster structures and collectivity, while such features are much more difficult using other methods. Furthermore it can be used to compute superfluid condensate fractions as well as the phase diagram of strongly matter and the density and temperature dependence of clustering. Lattice effective field theory was first used in simulations of infinite nuclear matter and infinite neutron matter with pions and without pions. In addition to the efforts by our collaboration, there have been recent efforts by other groups as well.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Diffusion quantum Monte Carlo approach to the polaritonic ground state

Making and using polaritonic states (i.e., hybrid electron-photon states) for chemical applications has recently become one of the most prominent and active fields that connects the communities of chemistry and quantum optics. Modeling of such polaritonic phenomena using ab initio approaches calls for new methodologies, leading to the reinvention of many commonly used electronic structure methods, such as Hartree-Fock, density functional, and coupled cluster theories. Here in this work, we explore the formally exact diffusion quantum Monte Carlo approach to obtain numerical solutions to the polaritonic ground state during the dissociation of the H 2 molecular system. Here, we examine various electron-nuclear-photon properties throughout the dissociation, such as changes to the minimum of the cavity Born-Oppenheimer surface, the localization of the electronic wave function, and the average mode occupation. Finally, we directly compare our results to that obtained with state-of-the-art, yet approximate, polaritonic coupled cluster approaches.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Quantification of electron correlation for approximate quantum calculations

State-of-the-art many-body wave function techniques rely on heuristics to achieve high accuracy at an attainable computational cost to solve the many-body Schrödinger equation. By far, the most common property used to assess accuracy has been the total energy; however, total energies do not give a complete picture of electron correlation. In this work, we assess the von Neumann entropy of the one-particle reduced density matrix (1-RDM) to compare selected configuration interaction (CI), coupled cluster, variational Monte Carlo, and fixed-node diffusion Monte Carlo for benchmark hydrogen chains. A new algorithm, the circle reject method, is presented, which improves the efficiency of evaluating the von Neumann entropy using quantum Monte Carlo by several orders of magnitude. The von Neumann entropy of the 1-RDM and the eigenvalues of the 1-RDM are shown to distinguish between the dynamic correlation introduced by the Jastrow and the static correlation introduced by determinants with large weights, confirming some of the lore in the field concerning the difference between the selected CI and Slater–Jastrow wave functions.

Chemistry↗
NASA NTRS2026

Diffusion Quantum Monte Carlo Calculation of the Austenite and Martensite Phases of NiTi

NiTi is a promising material for smart and active technologies due to its exhibition of the shape memory effect, superelasticity, and biocompatibility. The shape memory effect is tied to the reversible transition between the austenite and martensite phases. A major research direction is to alloy NiTi with Zr, Hf, Pd, Pt, etc., in order to tune the martensitic transition temperature (MTT). Modeling the MTT from first principles is challenging because the lattice dynamics is complicated by anharmonicity and various low-energy structures. Using density functional theory, the energy difference between the austenite and martensite phases of NiTi varies by up to 100 meV/atom depending on the choice of density functional, which is of the same order of the energy difference itself. Consequently, free energy calculations with different functionals can result in estimates of the MTT that vary by several hundred K. Using diffusion quantum Monte Carlo, we calculated the energy difference between the B2 and B19' structures of NiTi to be 70.9 +- 2.5 meV/atom.

Kevin K Ly↗
DOE OSTI2023

Stable Solid Molecular Hydrogen above 900 K from a Machine-Learned Potential Trained with Diffusion Quantum Monte Carlo

Here, we survey the phase diagram of high-pressure molecular hydrogen with path integral molecular dynamics using a machine-learned interatomic potential trained with quantum Monte Carlo forces and energies. Besides the HCP and C2/c–24 phases, we find two new stable phases both with molecular centers in the Fmmm–4 structure, separated by a molecular orientation transition with temperature. The high temperature isotropic Fmmm–4 phase has a reentrant melting line with a maximum at higher temperature (1450 K at 150 GPa) than previously estimated and crosses the liquid-liquid transition line around 1200 K and 200 GPa.

08 HYDROGEN↗
DOE OSTI2021

Origin of the $ν$ = 1/2 fractional quantum Hall effect in wide quantum wells

The nature of the fractional quantum Hall effect at ν = 1/2, observed in wide quantum wells al- most three decades ago, is still under debate. Previous studies have investigated it by the variational Monte Carlo method, which assumes that the transverse wave function and the gap between the symmetric and antisymmetric subbands obtained in a local density approximation at zero magnetic field remain valid even at high perpendicular magnetic fields; this method also ignores the effect of Landau level mixing. We develop in this work a three-dimensional fixed phase diffusion Monte Carlo method, which gives, in a single framework, the total energies of various candidate states in a finite width quantum well, including Landau level mixing, directly in a large magnetic field. This method can be applied to one-component states, and also to two-component states in the limit where the symmetric and antisymmetric bands are nearly degenerate. Our three-dimensional fixed-phase diffusion Monte Carlo calculations find that the one-component composite-fermion Fermi sea and the one-component Pfaffian states are very close in energy for a range of quantum well widths and densities, suggesting that the observed 1/2 fractional quantum Hall state in wide quantum wells is likely to be the one-component Pfaffian state. Furthermore, we hope that this will motivate further experimental studies of this state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Toward quantum Monte Carlo forces on heavier ions: Scaling properties

Quantum Monte Carlo (QMC) forces have been studied extensively in recent decades because of their importance with spectroscopic observables and geometry optimization. Here, we benchmark the accuracy and computational cost of QMC forces. The zero-variance zero-bias (ZVZB) force estimator is used in standard variational and diffusion Monte Carlo simulations with mean-field based trial wavefunctions and atomic pseudopotentials. Statistical force uncertainties are obtained with a recently developed regression technique for heavy tailed QMC data [P. Lopez Rios and G. J. Conduit, Phys. Rev. E 99, 063312 (2019)]. By considering selected atoms and dimers with elements ranging from H to Zn (1 ≤ Z eff ≤ 20), we assess the accuracy and the computational cost of ZVZB forces as the effective pseudopotential valence charge, Z eff , increases. We find that the costs of QMC energies and forces approximately follow simple power laws in Zeff. The force uncertainty grows more rapidly, leading to a best case cost scaling relationship of approximately Z e ff 6.5 ( 3 ) for diffusion Monte Carlo. We find that the accessible system size at fixed computational cost scales as Z e ff − 2 , insensitive to model assumptions or the use of the “space warp” variance-reduction technique. Our results predict the practical cost of obtaining forces for a range of materials, such as transition metal oxides where QMC forces have yet to be applied, and underscore the importance of further developing force variance-reduction techniques, particularly for atoms with high Z eff .

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

Maximally local two-nucleon interactions at N 3 LO in Δ -less chiral effective field theory

We present new maximally local two-nucleon interactions derived in Δ -less chiral effective field theory up to next-to-next-to-next-to-leading order ( N 3 LO ), which include all contact and pion-exchange contributions to the nuclear Hamiltonian up to this order. Our interactions are fit to nucleon-nucleon phase shifts using a Bayesian statistical approach, and explore a wide cutoff range from 0.6 – 0.9 fm ( ≈ 660 – 440 MeV ). These interactions can be straightforwardly employed in quantum Monte Carlo methods, such as the auxiliary field diffusion Monte Carlo method. Together with local three-nucleon forces, calculations with these new interactions will provide improved benchmarks for the structure of atomic nuclei and serve as crucial input to analyses of astrophysical phenomena of neutron stars, such as binary neutron-star mergers. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Static and dynamic properties of atomic nuclei with high-resolution potentials

Here, we compute ground-state and dynamical properties of 4 He and 16 O nuclei using as input high-resolution, phenomenological nucleon-nucleon and three-nucleon forces that are local in coordinate space. The nuclear Schrodinger equation for both nuclei is accurately solved employing the auxiliary-field diffusion Monte Carlo approach. For the 4 He nucleus, detailed benchmarks are carried out with the hyperspherical harmonics method. In addition to presenting results for the binding energies and radii, we also analyze the momentum distributions of these nuclei and their Euclidean response function corresponding to the isoscalar density transition. The latter quantity is particularly relevant for lepton-nucleus scattering experiments, as it paves the way to quantum Monte Carlo calculations of electroweak response functions of 16 O.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Benchmark calculations of pure neutron matter with realistic nucleon-nucleon interactions

Here, we report benchmark calculations of the energy per particle of pure neutron matter as a function of the baryon density using three independent many-body methods: Brueckner–Bethe–Goldstone, Fermi hypernetted chain/single-operator chain, and auxiliary-field diffusion Monte Carlo. Significant technical improvements are implemented in the latter two methods. The calculations are made for two distinct families of realistic coordinate-space nucleon-nucleon potentials fit to scattering data, including the standard Argonne v 18 interaction and two of its simplified versions, and four of the new Norfolk Δ -full chiral effective field theory potentials. Primarily because of the advancements in the auxiliary-field diffusion Monte Carlo, we observe good agreement among the three many-body techniques up to nuclear saturation density—the maximum difference in the energy per particle is within 1.5 MeV for all the potentials we consider. At higher densities, the divergences become more important, and are mainly driven by the Fermi hypernetted chain/single-operator calculations. We also study the connection between nucleon-nucleon scattering data and the energy per particle of pure neutron matter. Our results suggest that fitting to higher-energy nucleon-nucleon scattering helps reduce the spread of energies among the models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

QMCPACK: Advances in the development, efficiency, and application of auxiliary field and real-space variational and diffusion quantum Monte Carlo

We review recent advances in the capabilities of the open source ab initio Quantum Monte Carlo (QMC) package QMCPACK and the workflow tool Nexus used for greater efficiency and reproducibility. The auxiliary field QMC (AFQMC) implementation has been greatly expanded to include k-point symmetries, tensor-hypercontraction, and accelerated graphical processing unit (GPU) support. These scaling and memory reductions greatly increase the number of orbitals that can practically be included in AFQMC calculations, increasing the accuracy. Advances in real space methods include techniques for accurate computation of bandgaps and for systematically improving the nodal surface of ground state wavefunctions. Results of these calculations can be used to validate application of more approximate electronic structure methods, including GW and density functional based techniques. To provide an improved foundation for these calculations, we utilize a new set of correlation-consistent effective core potentials (pseudopotentials) that are more accurate than previous sets; these can also be applied in quantum-chemical and other many-body applications, not only QMC. These advances increase the efficiency, accuracy, and range of properties that can be studied in both molecules and materials with QMC and QMCPACK.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Systematic correction of the density functional theory spectra via a quantum Monte Carlo approach

Numerical outputs and driver scripts supporting auxiliary-boson corrected diffusion Monte Carlo (ABCDMC) benchmarks on second-row neutral atoms, cations, and dications, plus a C2 molecule active-space study. Includes NIST reference energies, ABCDMC timestep extrapolation summaries, orbital generation inputs, singles-only CASCI driver scripts, an O-atom basis-set convergence study, and the PyQMC boson code snapshot used for the calculations.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A quantum Monte Carlo study of systems with effective core potentials and node nonlinearities

In this report we study beryllium dihydride (BeH2) and acetylene (C2H2) molecules using real-space diffusion Monte Carlo (DMC) method. The molecules serve as perhaps the simplest prototypes that illustrate the difficulties with biases in the fixed-node DMC calculations that might appear with the use of effective core potentials (ECPs) or other nonlocal operators. This is especially relevant for the recently introduced correlation consistent ECPs (ccECPs) for 2s2p elements. Corresponding ccECPs exhibit deeper potential functions due to higher fidelity to all-electron counterparts, which could lead to larger local energy fluctuations. We point out that the difficulties stem from issues that are straightforward to address by upgrades of basis sets, use of T-moves for nonlocal terms, inclusion of a few configurations into the trial function and similar. The resulting accuracy corresponds to the ccECP target (chemical accuracy) and it is in consistent agreement with independent correlated calculations. Further possibilities for upgrading the reliability of the DMC algorithm and considerations for better adapted and more robust Jastrow factors are discussed as well.

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

Competition between Hückel’s Rule and Jahn–Teller Distortion in Small Carbon Rings: A Quantum Monte Carlo Study

Structural properties and energetics of carbon rings are studied with the diffusion Monte Carlo (DMC) method. Our DMC-based geometry optimization reveals that both polyynic C 4n and cumulenic C 4n+2 rings exhibit bond length alternations for n >= 3, which is understood to be due to Jahn-Teller distortions. The bond length alternation even in a cumulenic (4n + 2) carbon ring was experimentally observed in a recently synthesized C 18 molecule. From a comparison of the DMC cohesive energies of C 4n with those of C 4n + 2 , we present a comprehensive picture of the competition between Huckel's rule and Jahn-Teller distortion in small carbon rings; the former is more dominant than the latter for n < 5 where C 4n + 2 rings are more stable than C 4n , while C 4n rings are as stable as C 4n + 2 for n < 5 where dimerization effects due to Jahn-Teller distortion are more important.

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

Quantum Monte Carlo benchmarking of large noncovalent complexes in the L7 benchmark set

We have used diffusion Monte Carlo (DMC) to perform calculations on the L7 benchmark set. DMC is a stochastic numerical integration scheme in real-space and part of a larger set of quantum Monte Carlo methods. The L7 set was designed to test the ability of electronic structure methods to include dispersive interactions. While the agreement between DMC and quantum-chemical state-of-the-art methods is excellent for some of the structures, there are significant differences in others. In contrast to wavefunction-based quantum chemical methods, DMC is a first-principle many-body method with the many-body wavefunction evolving in real space. It includes explicitly all electron–electron interactions and is relatively insensitive to the size of the basis set.

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

Spin Susceptibility in Neutron Matter from Quantum Monte Carlo Calculations

The spin susceptibility in pure neutron matter is computed from auxiliary field diffusion Monte Carlo calculations over a wide range of densities. The calculations are performed for different spin asymmetries, while using twist-averaged boundary conditions to reduce finite-size effects. The employed nuclear interactions include both the phenomenological Argonne AV8′ + UIX potential and local interactions that are derived from chiral effective field theory up to next-to-next-to-leading order.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗