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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Quantum computing and quantum information storage

Quantum storage, transmission, and processing is the future of information technology. Here, the promise of quantum hardware stems from the inherent complexity of an entangled quantum system—the size of the wave-function scales exponentially with the number of particles, whether represented in real space or in a parameter space. In contrast, a classical N-body system can be completely represented by only 6N variables (positions and momenta of all particles). This complexity of quantum systems creates a yet-unsolved challenge of modeling quantum systems by means of classical computing—the curse of dimensionality. Indeed, although we can easily write the Schrödinger equation for any system of interacting nuclei and electrons, we can only solve it exactly on classical computers for very small systems.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2020

Extension of frozen natural orbital approximation to open-shell references: Theory, implementation, and application to single-molecule magnets

Natural orbitals are often used to achieve a more compact representation of correlated wave-functions. Using natural orbitals computed as eigenstates of the virtual–virtual block of the state density matrix instead of the canonical Hartree–Fock orbitals results in smaller errors when the same fraction of virtual space is frozen. This strategy, termed frozen natural orbital (FNO) approach, is effective in reducing the cost of regular coupled-cluster (CC) calculations and some multistate methods, such as EOM-IP-CC (equation-of-motion CC for ionization potentials). This contribution extends the FNO approach to the EOM-SF-CC ansatz (EOM-CC with spin-flip). In contrast to EOM-IP-CCSD, EOM-SF-CCSD relies on high-spin open-shell references. Using FNOs computed for an open-shell reference leads to an erratic behavior of the EOM-SF-CC energies and properties due to an inconsistent truncation of the α and β orbital spaces. A general solution to problems arising in the EOM-CC calculations utilizing open-shell references, termed OSFNO (open-shell FNO), is proposed. Furthermore, by means of singular value decomposition (SVD) of the overlap matrix of the α and β orbitals, the OSFNO algorithm identifies the corresponding orbitals and determines virtual orbitals corresponding to the singly occupied space. This is followed by SVD of the singlet part of the state density matrix in the remaining virtual orbital subspace. The so-computed FNOs preserve the spin purity of the open-shell orbital subspace to the extent allowed by the original reference, thus facilitating a safe truncation of the virtual space. The performance of OSFNO is benchmarked for selected diradicals and triradicals.

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

GPAW: An open Python package for electronic structure calculations

We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for the implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE), providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe–Salpeter Equation, variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn–Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support for graphics processing unit (GPU) acceleration has been achieved with minor modifications to the GPAW code thanks to the CuPy library. We end the review with an outlook, describing some future plans for GPAW.

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

Non-relativistic geometry and the equivalence principle

Abstract We describe a geometric and symmetry-based formulation of the equivalence principle in non-relativistic physics. It applies both on the classical and quantum levels and states that the Newtonian potential can be eliminated in favor of a curved and time-dependent spatial metric. It is this requirement that forces the gravitational mass to be equal to the inertial mass. We identify the symmetry responsible for the equivalence principle as the remnant of time-reparameterization symmetry of the relativistic theory. We also clarify the transformation properties of the Schrödinger wave-function under arbitrary frame changes.

Astronomy & Astrophysics↗
DOE OSTI2024

Roadmap on methods and software for electronic structure based simulations in chemistry and materials

This Roadmap article provides a succinct, comprehensive overview of the state of electronic structure methods and software for molecular and materials simulations. Seventeen distinct sections collect insights by 51 leading scientists in the field. Each contribution addresses the status of a particular area, as well as current challenges and anticipated future advances, with a particular eye towards software related aspects and providing key references for further reading. Foundational sections cover density functional theory and its implementation in real-world simulation frameworks, Green's function based many-body perturbation theory, wave-function based and stochastic electronic structure approaches, relativistic effects and semiempirical electronic structure theory approaches. Subsequent sections cover nuclear quantum effects, real-time propagation of the electronic structure, challenges for computational spectroscopy simulations, and exploration of complex potential energy surfaces. The final sections summarize practical aspects, including computational workflows for complex simulation tasks, the impact of current and future high-performance computing architectures, software engineering practices, education and training to maintain and broaden the community, as well as the status of and needs for electronic structure based modeling from the vantage point of industry environments. Overall, the field of electronic structure software and method development continues to unlock immense opportunities for future scientific discovery, based on the growing ability of computations to reveal complex phenomena, processes and properties that are determined by the make-up of matter at the atomic scale, with high precision.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Filtering states with total spin on a quantum computer

Starting from a general wave-function described on a set of spins or qubits, we propose several quantum algorithms to extract the components of this state on eigenstates of total spin S 2 and its z component S z . The method plays the role of total spin projection and gives access to the amplitudes of the initial state on a total spin basis. Here, the different algorithms have various degrees of sophistication depending on the requested tasks. They can either solely project onto the subspace with good total spin or completely uplift the degeneracy in this subspace. In the former case, when the projection on the total spin j is made, we show that the number of operations for the projection can be reduced from a quadratic to a linear dependence in j. After each measurement, the state collapses to one of the spin eigenstates that could be used for postprocessing. For this reason, we call the method total quantum spin filtering.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Quantum Monte Carlo determination of the principal Hugoniot of deuterium

Here, we present coupled electron-ion Monte Carlo results for the principal Hugoniot of deuterium together with an accurate study of the initial reference state of shock-wave experiments. We discuss the influence of nuclear quantum effects, thermal electronic excitations, and the convergence of the potential energy surface by wave-function optimization within variational Monte Carlo and projection quantum Monte Carlo methods. Compared to a previous study, our calculations also include low pressure-temperature (P,T) conditions resulting in close agreement with experimental data, while our revised results at higher (P,T) conditions still predict a more compressible Hugoniot than experimentally observed.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Charge ordering in Ir dimers in the ground state of Ba 5 AlIr 2 O 11

It has been well established experimentally that the interplay of electronic correlations and spin-orbit interactions in Ir 4+ and Ir 5+ oxides results in insulating J eff = 1/2 and J eff = 0 ground states, respectively. However, in compounds where the structural dimerization of iridium ions is favorable, the direct Ir d-d hybridization can be significant and takes a key role. Here, in this study, we investigate the effects of direct Ir d-d hybridization in comparison with electronic correlations and spin-orbit coupling in Ba 5 AlIr 2 O 11 , a compound with Ir dimers. Using a combination of ab initio many-body wave-function quantum chemistry calculations and resonant inelastic x-ray scattering experiments, we elucidate the electronic structure of Ba 5 AlIr 2 O 11 . We find excellent agreement between the calculated and the measured spin-orbit excitations. Contrary to expectations, the analysis of the many-body wave function shows that the two Ir (Ir 4+ and Ir 5+ ) ions in the Ir 2 O 9 dimer unit in this compound preserve their local J eff character close to 1/2 and 0, respectively. The local point group symmetry at each of the Ir ions plays an important role, significantly limiting the direct d-d hybridization. Our results emphasize that minute details in the local crystal field environment can lead to dramatic differences in the electronic states in iridates and 5d oxides in general.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Orbital design of flat bands in non-line-graph lattices via line-graph wave functions

Line-graph (LG) lattices are known for having flat bands (FBs) from the destructive interference of Bloch wave functions encoded in only lattice symmetry. In this work, we develop a generic atomic/molecular orbital design principle for FBs in non-LG lattices. Based on linear combination of atomic orbital theory, we demonstrate that the underlying wave-function symmetry of FBs in a LG lattice can be transformed into the atomic/molecular orbital symmetry in a non-LG lattice. We illustrate such orbital-designed topological FBs in three 2D non-LG, square, trigonal, and hexagonal lattices, where the designed orbitals faithfully reproduce the corresponding lattice symmetries of checkerboard, kagome, and diatomic-kagome lattices, respectively. Interestingly, systematic design of FBs with a high Chern number is also achieved based on the same principle. Fundamentally our theory enriches the FB physics; practically, it significantly expands the scope of FB materials, since most materials have multiple atomic/molecular orbitals at each lattice site, rather than a single s orbital mandated in graph theory and generic lattice models.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Random insights into the complexity of two-dimensional tensor network calculations

Projected entangled pair states (PEPS) offer memory-efficient representations of some quantum many-body states that obey an entanglement area law and are the basis for classical simulations of ground states in two-dimensional (2d) condensed matter systems. However, rigorous results show that exactly computing observables from a 2d PEPS state is generically a computationally hard problem. Yet approximation schemes for computing properties of 2d PEPS are regularly used, and empirically seen to succeed, for a large subclass of (“not too entangled”) condensed matter ground states. Adopting the philosophy of random matrix theory, in this work, we analyze the complexity of approximately contracting a 2d random PEPS by exploiting an analytic mapping to an effective replicated statistical mechanics model that permits a controlled analysis at a large bond dimension. Through this statistical-mechanics lens, we argue that (i) although approximately sampling wave-function amplitudes of random PEPS faces a computational-complexity phase transition above a critical bond dimension, and (ii) one can generically efficiently estimate the norm and correlation functions for any finite bond dimension. Furthermore, these results are supported numerically for various bond-dimension regimes. It is an important open question whether the above results for random PEPS apply more generally also to PEPS representing physically relevant ground states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Updated systematics of intermediate-energy single-nucleon removal cross sections

The body of experimental measurements of intermediate-energy reactions that remove a single nucleon from a secondary beam of neutron- or proton-rich nuclei continues to grow. These data have been analyzed consistently using an approximate, eikonal-model treatment of the reaction dynamics combined with appropriate shell-model descriptions of the projectile initial state, the bound final states spectrum of the reaction residue, and single-particle removal strengths computed from their wave-function overlaps. Here, the systematics of the ratio R s of the measured inclusive cross section to all bound final states and the calculated cross section to bound shell-model states—in different regions of the nuclear chart and involving both very weakly bound and strongly bound valence nucleons—is important in relating the empirically deduced orbital occupancies to those from the best available shell-model predictions. Importantly, several new higher-energy measurements, for which the sudden-approximation aspect of the dynamical description is placed on an even stronger footing, now supplement the previously analyzed measurements. These additional data sets are discussed. Their R s values are shown to conform to and reinforce the earlier-observed systematics, with no indication that the approximately linear reduction in R s with increasing nucleon separation energy is a consequence of a breakdown of the sudden approximation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Short-range correlation physics at low renormalization group resolution

Recent experiments have succeeded in isolating processes for which short-range correlation (SRC) physics is dominant and well accounted for by SRC phenomenology. But an alternative and compelling picture emerges from renormalization group (RG) evolution to low RG resolution. At high RG resolution, SRCs are identified as components in the nuclear wave function with relative pair momenta greater than the Fermi momentum. Scale separation results in wave-function factorization that can be exploited with phenomenologies such as the generalized contact formalism or the low-order correlation operator approximation. Evolution to lower resolution shifts SRC physics from nuclear structure to the reaction operators without changing the measured observables. We show how the features of SRC phenomenology manifested at high RG resolution are cleanly identified at low RG resolution using simple two-body operators and local-density approximations with uncorrelated wave functions, all of which can be systematically generalized. We verify that the experimental consequences to date follow directly at low resolution from well-established properties of nucleon-nucleon interactions such as the tensor force. Thus the RG reconciles the contrasting pictures of the same experiment and shows how to get correct results using wave functions without SRC components. Finally, our demonstration has implications for the analysis of knockout reactions for which SRC physics is not cleanly isolated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Alternative to perturbative renormalization in ( 3 + 1 )-dimensional field theories

Perturbative renormalization provides the bedrock of understanding quantum field theories. In this work, I point out an alternative way of renormalizing quantum field theories, which is naturally encountered and well-known for the case of large N scalar field theories. In terms of bare parameters, this nonperturbative alternative renormalization differs qualitatively from its perturbative cousin: in the continuum limit, the bare coupling constant goes to zero instead of infinity, and there is no wave-function counterterm. Despite these differences, the resulting n -point functions of the theory are finite. I provide explicit results for alternative renormalization for the O(N) model and QCD with N f = 12 flavors in 3 + 1 dimensions. Published by the American Physical Society 2024

Astronomy & Astrophysics↗
DOE OSTI2021

Distinct critical behaviors from the same state in quantum spin and population dynamics perspectives

There is a deep connection between the ground states of transverse-field spin systems and the late-time distributions of evolving viral populations—within simple models, both are obtained from the principal eigenvector of the same matrix. However, that vector is the wave-function amplitude in the quantum spin model, whereas it is the probability itself in the population model. We show that this seemingly minor difference has significant consequences: Phase transitions that are discontinuous in the spin system become continuous when viewed through the population perspective, and transitions that are continuous become governed by new critical exponents. We introduce a more general class of models that encompasses both cases and that can be solved exactly in a mean-field limit. Numerical results are also presented for a number of one-dimensional chains with power-law interactions. We see that well-worn spin models of quantum statistical mechanics can contain unexpected new physics and insights when treated as population-dynamical models and beyond, motivating further studies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Mixed excitonic nature in water-oxidized BiVO 4 surfaces with defects

BiVO 4 is a promising photocatalyst for efficient water oxidation, with surface reactivity determined by the structure of active catalytic sites. Surface oxidation in the presence of oxygen vacancies induces electron localization, suggesting an atomistic route to improve the charge transfer efficiency within the catalytic cycle. In this paper, we study the effect of oxygen vacancies on the electronic and optical properties at BiVO 4 surfaces upon water oxidation. We use density functional theory and many-body perturbation theory to explore the change in the electronic and quasiparticle energy levels and to evaluate the electron-hole coupling as a function of the underlying structure. Further we show that while the presence of defects alters the atomic structure and largely modifies the wave-function nature, leading to defect-localized states at the quasiparticle gap region, the optical excitations remain largely unchanged due to the substantial hybridization of defect and nondefect electron-hole transitions. Our findings suggest that defect-induced surface oxidation supports improved electron transport, both through bound and tunable electronic states and via a mixed nature of the optical transitions, expected to reduce electron-hole defect trapping.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Exact block encoding of imaginary time evolution with universal quantum neural networks

We develop a constructive approach to generate quantum neural networks capable of representing the exact thermal states of all many-body qubit Hamiltonians. The Trotter expansion of the imaginary time propagator is implemented through an exact block encoding by means of a unitary, restricted Boltzmann machine architecture. Marginalization over the hidden-layer neurons (auxiliary qubits) creates the nonunitary action on the visible layer. Then, we introduce a unitary deep Boltzmann machine architecture in which the hidden-layer qubits are allowed to couple laterally to other hidden qubits. We prove that this wave-function is closed under the action of the imaginary time propagator and, more generally, can represent the action of a universal set of quantum gate operations. We provide analytic expressions for the coefficients for both architectures, thus enabling exact network representations of thermal states without stochastic optimization of the network parameters. In the limit of large imaginary time, the yields the ground state of the system. The number of qubits grows linearly with the number of interactions and total imaginary time for a fixed interaction order. Both networks can be readily implemented on quantum hardware via midcircuit measurements of auxiliary qubits. If only one auxiliary qubit is measured and reset, the circuit depth scales linearly with imaginary time and number of interactions, while the width is constant. Alternatively, one can employ a number of auxiliary qubits linearly proportional to the number of interactions, and circuit depth grows linearly with imaginary time only. Every midcircuit measurement has a postselection success probability, and the overall success probability is equal to the product of the probabilities of the midcircuit measurements.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2025

Kolmogorov-Arnold wavefunctions

Here, this work investigates Kolmogorov-Arnold network-based (KAN) wave-function Ansätz as viable representations for quantum Monte Carlo simulations. Through systematic analysis of one-dimensional model systems, we evaluate their computational efficiency and representational power against established methods. Our numerical experiments suggest some efficient training methods and we explore how the computational cost scales with desired precision, particle number, and system parameters. Roughly speaking, KANs seem to be 10 times cheaper computationally than other neural-network-based Ansätz . We also introduce a novel approach for handling strong short-range potentials—a persistent challenge for many numerical techniques—which generalizes efficiently to higher-dimensional, physically relevant systems with short-ranged strong potentials common in atomic and nuclear physics.

1-dimensional systems↗
DOE OSTI2024

Breaking the Million-Electron and 1 EFLOP/s Barriers: Biomolecular-Scale Ab Initio Molecular Dynamics Using MP2 Potentials

The accurate simulation of complex biochemical phenomena has historically been hampered by the computational requirements of high-fidelity molecular-modeling techniques. Quantum mechanical methods, such as ab initio wave-function (WF) theory, deliver the desired accuracy, but have impractical scaling for modeling biosystems with thousands of atoms. Combining molecular fragmentation with MP2 perturbation theory, this study presents an innovative approach that enables biomolecular-scale ab initio molecular dynamics (AIMD) simulations at WF theory level. Leveraging the resolution-of-the-identity approximation for Hartree-Fock and MP2 gradients, our approach eliminates computationally intensive four-center integrals and their gradients, while achieving near-peak performance on modern GPU architectures. The introduction of asynchronous time steps minimizes time step latency, overlapping computational phases and effectively mitigating load imbalances. Utilizing up to 9,400 nodes of Frontier and achieving 59% (1006.7 PFLOP/s) of its double-precision floating-point peak, our method enables us to break the million-electron and 1EFLOP/s barriers for AIMD simulations with quantum accuracy.

Kurzak, Jakub↗