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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

The future of the correlated electron problem

A central problem in modern condensed matter physics is the understanding of materials with strong electron correlations. Despite extensive work, the essential physics of many of these systems is not understood and there is very little ability to make predictions in this class of materials. In this manuscript we share our personal views on the major open problems in the field of correlated electron systems. We discuss some possible routes to make progress in this rich and fascinating field. This manuscript is the result of the vigorous discussions and deliberations that took place at Johns Hopkins University during a three-day workshop January 27, 28, and 29, 2020 that brought together six senior scientists and 46 more junior scientists. Our hope, is that the topics we have presented will provide inspiration for others working in this field and motivation for the idea that significant progress can be made on very hard problems if we focus our collective energies.

Alexandradinata, Aris [Univ. of Illinois at Urbana↗
DOE OSTI2025

Multireference diffusion Monte Carlo reaches 2D materials

Abstract Quantum confinement in 2D materials strongly enhances electronic correlation effects. Therefore, predicting the properties of these unique materials, with both a high level of accuracy and computational efficiency, without relying on adjustable parameters or functionals, remains an outstanding theoretical challenge. The majority of theoretical studies are based on the approximations of density functional theory (DFT). The reliability of DFT predictions are heavily dependent on the choice of an approximated exchange-correlation functional. Here, we estimate the magnitude of impact of correlation on the total energy for the quintessential 2D material, graphene, by performing and comparing state-of-the-art selected CI and quantum Monte Carlo extrapolated calculations for a single unit cell at the$$\Gamma$$point. We demonstrate that Self-Healing Diffusion Monte Carlo (SHDMC) obtains a very compact, but high-quality wavefunction for this system that lacks the strong basis set dependence displayed by state of the art quantum chemistry methods. The SHDMC wavefunction is of higher quality compared to that obtained from sCI, in the same orbital basis, while being$$\sim$$ 1000 times smaller in terms of determinant count compared to sCI. We also demonstrate that extrapolating SHDMC results to the infinite determinant limit compares extremely well with complete basis set extrapolated sCI. Our work paves the way for future validation of SHDMC applied to challenging 2D materials.

Science & Technology - Other Topics↗
DOE OSTI2020

Quantum Matter: Computation Meets Experiments

The past few years have seen tremendous advances in our understanding of strongly interacting quantum systems. By combining progress in theoretical concepts and methods with algorithmic advances, computational methods have shed new light on key open questions in the physics of quantum matter, both for materials with strong electronic correlations and for interacting quantum gases. At the same time, new materials and new techniques have greatly increased the range of experimental information available. This Aspen Winter Conference will bring leading theorists with expertise in a broad range of computational methods together with experimentalists to discuss the potential of new methods, the accomplishments of existing methods and opportunities for future experiment/ theory collaboration. The meeting will focus on a broad set of physics questions of current interest in the field, for which computational methods and experiments have brought or have the potential to bring new insights.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Effects of Photovoltaic Module Materials and Design on Module Deformation Under Load

Quasi-static structural finite-element models of an aluminum-framed crystalline silicon photovoltaic module and a glass-glass thin-film module were constructed and validated against experimental measurements of deflection under uniform pressure loading. Specific practices in the computational representation of module assembly were identified as influential to matching experimental deflection observations. Additionally, parametric analyses using Latin hypercube sampling were performed to propagate input uncertainties related to module materials, dimensions, and tolerances into uncertainties in simulated deflection. Sensitivity analyses were performed on the uncertainty quantification datasets using linear correlation coefficients and variance-based sensitivity indices to elucidate key parameters influencing module deformation. Results identified edge tape and adhesive material properties as being strongly correlated to module deflection, suggesting that optimization of these materials could yield module stiffness gains at par with the conventionally structural parameters, such as glass thickness. This exercise verifies the applicability of finite-element models for accurately predicting mechanical behavior of solar modules and demonstrates a workflow for model-based parametric uncertainty quantification and sensitivity analysis. Finally, applications of this capability include the assessment of field environment loads, derivation of representative loading conditions for reduced-scale testing, and module design optimization, among others.

42 ENGINEERING↗
DOE OSTI2021

Engineering of Ferroic Orders in Thin Films by Anionic Substitution

Multiferroics are a unique class of materials where magnetic and ferroelectric orders coexist. The research on multiferroics contributes significantly to the fundamental understanding of the strong correlations between different material degrees of freedom and provides an energy-efficient route toward the electrical control of magnetism. While multiple ABO 3 oxide perovskites are identified as being multiferroic, their magnetoelectric coupling strength is often weak, necessitating the material search in different compounds. Here, the observation of room-temperature multiferroic orders in multi-anion SrNbO 3-x N x thin films is reported. In these samples, the multi-anion state enables the room-temperature ferromagnetic ordering of the Nb d-electrons. Simultaneously, ferroelectric responses that originate from the structural symmetry breaking associated are found with both the off-center displacements of Nb and the geometric displacements of Sr, depending on the relative O-N arrangements within the Nb-centered octahedra. So findings not only diversify the available multiferroic material pool but also demonstrate a new multiferroism design strategy via multi-anion engineering.

thin-films↗
DOE OSTI2021

Realization of Electron Antidoping by Modulating the Breathing Distortion in BaBiO 3

The recent proposal of antidoping scheme breaks new ground in conceiving conversely functional materials and devices; yet, the few available examples belong to the correlated electron systems. Here, we demonstrate both theoretically and experimentally that the main group oxide BaBiO 3 is a model system for antidoping using oxygen vacancies. The first-principles calculations show that the band gap systematically increases due to the strongly enhanced Bi-O breathing distortions away from the vacancies and the annihilation of Bi 6 s /O 2 p hybridized conduction bands near the vacancies. Our further spectroscopic experiments confirm that the band gap increases systematically with electron doping, with a maximal gap enhancement of ~75% when the film's stoichiometry is reduced to BaBiO 2.75 . These results unambiguously demonstrate the remarkable antidoping effect in a material without strong electron correlations and underscores the importance of bond disproportionation in realizing such an effect.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Low-temperature emergent neuromorphic networks with correlated oxide devices

Significance Designing neuromorphic hardware for cryoelectronics is an important area of research as the field of computing paradigms beyond complementary metal-oxide-semiconductor (CMOS) progresses. Superconductivity and metal−insulator transitions are two of the most celebrated emergent, collective properties found in quantum materials such as strongly correlated oxides. Here, we present simulations of artificial neural networks that can be designed by combining superconducting devices (e.g. Josephson junctions) with Mott metal−insulator transition−based tunable resistor devices. Our simulations show that 1) neurons and synapses can be seamlessly created, 2) their functions can be tuned via learning, and 3) controlling disorder by incorporating light ions enables exponential multiplicity of states. The results open up directions for incorporating emergent behavior seen in condensed matter into hardware design for artificial intelligence.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2021

Angle-resolved photoemission studies of quantum materials

The physics of quantum materials is dictated by many-body interactions and mathematical concepts such as symmetry and topology that have transformed our understanding of matter. Angle-resolved photoemission spectroscopy (ARPES), which directly probes the electronic structure in momentum space, has played a central role in the discovery, characterization, and understanding of quantum materials ranging from strongly correlated states of matter to those exhibiting nontrivial topology. Over the past two decades, ARPES as a technique has matured dramatically with ever-improving resolution and continued expansion into the space, time, and spin domains. Simultaneously, the capability to synthesize new materials and apply nonthermal tuning parameters in situ has unlocked new dimensions in the study of all quantum materials. These developments are reviewed, and the scientific contributions they have enabled in contemporary quantum materials research are surveyed.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Modulating Oxide‐Based Quantum Materials by Ion Implantation

Ion implantation has emerged as a powerful tool for manipulating and investigating oxide quantum materials, where strong electron correlations give rise to exotic phases and functionalities. This Review examines how controlled ion bombardment enables targeted modulation of structural, electronic, and magnetic properties in complex oxides. Recent advances in ion beam techniques is analyzed that provide unprecedented control over defect profiles, from point defects to extended damage cascades. In application, ion irradiation has demonstrated the ability to tune quantum phenomena including metal‐insulator transitions, magnetism, and superconductivity through selective doping, defect creation, and lattice strain. The ability to write quantum states with nanoscale precision using focused ion beams is opening new paths for quantum device fabrication. Challenges in understanding radiation damage mechanisms in strongly correlated systems is discussed, and identify opportunities for designing quantum functionality through defect‐engineering approaches. The technique's demonstrated capability to write quantum states with nanoscale precision, combined with its compatibility with existing semiconductor processing infrastructure, suggests a clear pathway for translating fundamental discoveries in quantum materials into practical technological applications.

defect engineering↗
DOE OSTI2024

Valley-Coherent Quantum Anomalous Hall State in AB-Stacked MoTe 2 / W S e 2 Bilayers

Moiré materials provide fertile ground for the correlated and topological quantum phenomena. Among them, the quantum anomalous Hall (QAH) effect, in which the Hall resistance is quantized even under zero magnetic field, is a direct manifestation of the intrinsic topological properties of a material and an appealing attribute for low-power electronics applications. The QAH effect has been observed in both graphene and transition metal dichalcogenide (TMD) moiré materials. It is thought to arise from the interaction-driven valley polarization of the narrow moiré bands. Here, we show that the newly discovered QAH state in AB-stacked MoTe 2 / W S e 2 moiré bilayers is not valley polarized but valley coherent. The layer- and helicity-resolved optical spectroscopy measurement reveals that the QAH ground state possesses spontaneous spin (valley) polarization aligned (antialigned) in two TMD layers. In addition, saturation of the out-of-plane spin polarization in both layers occurs only under high magnetic fields, supporting a canted spin texture. Our results call for a new mechanism for the QAH effect and highlight the potential of TMD moiré materials with strong electronic correlations and spin-orbit interactions for exotic topological states. Published by the American Physical Society 2024

2-dimensional systems↗
DOE OSTI2020

A non-orthogonal variational quantum eigensolver

Variational algorithms for strongly correlated chemical and materials systems are one of the most promising applications of near-term quantum computers. We present an extension to the variational quantum eigensolver that approximates the ground state of a system by solving a generalized eigenvalue problem in a subspace spanned by a collection of parametrized quantum states. This allows for the systematic improvement of a logical wavefunction ansatz without a significant increase in circuit complexity. To minimize the circuit complexity of this approach, we propose a strategy for efficiently measuring the Hamiltonian and overlap matrix elements between states parametrized by circuits that commute with the total particle number operator. This strategy doubles the size of the state preparation circuits but not their depth, while adding a small number of additional two-qubit gates relative to standard variational quantum eigensolver. We also propose a classical Monte Carlo scheme to estimate the uncertainty in the ground state energy caused by a finite number of measurements of the matrix elements. We explain how this Monte Carlo procedure can be extended to adaptively schedule the required measurements, reducing the number of circuit executions necessary for a given accuracy. We apply these ideas to two model strongly correlated systems, a square configuration of H4 and the π-system of hexatriene (C6H8).

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Spin-triplet pairing induced by near-neighbor attraction in the extended Hubbard model for cuprate chain

Abstract In quantum materials, the electronic interaction and the electron-phonon coupling are, in general, two essential ingredients, the combined impact of which may drive exotic phases. Recently, an anomalously strong electron-electron attraction, likely mediated by phonons, has been proposed in one-dimensional copper-oxide chain Ba 2− x Sr x CuO 3+ δ . Yet, it is unclear how this strong near-neighbor attraction V influences the superconductivity pairing in the system. Here we perform accurate many-body calculations to study the extended Hubbard model with on-site Coulomb repulsion U > 0 and near-neighbor attraction V < 0 that could well describe the cuprate chain and likely other similar transition-metal materials with both strong correlations and lattice effects. We find a rich quantum phase diagram containing an intriguing Tomonaga-Luttinger liquid phase — besides the spin density wave and various phase separation phases — that can host dominant spin-triplet pairing correlations and divergent superconductive susceptibility. Upon doping, the spin-triplet superconducting regime can be further broadened, offering a feasible mechanism to realize p -wave superconductivity in realistic cuprate chains.

36 MATERIALS SCIENCE↗
DOE OSTI2026

A statistical approach to analyzing domain dynamics in ferroelectric crystals using X-ray photon correlation spectroscopy

Ferroelectric materials exhibit strong electromechanical coupling, largely influenced by their domain structures. Numerous microstructural studies indicate that smaller domains with higher domain wall density generally enhance domain wall motion, although some inconsistencies have been reported. In this work, we use X-ray photon correlation spectroscopy (XPCS) to probe dynamic response in Pb(Mg 1/3 Nb 2/3 )O 3 -29PbTiO 3 (PMN-29PT) single crystals under applied electric fields. We introduce a two-field correlation approach, adapted from conventional two-time correlation to quantify dynamics. Statistical analysis reveals that both [001]-oriented direct current (DC) and alternating current (AC) poled samples show Poisson-like behavior within specific electric field regions. The DC-poled samples exhibit more frequent domain wall jump events but with smaller amount of decorrelation per jump event, whereas the AC-poled samples show fewer jump events with larger decorrelation per jump event. This observation aligns with the prevalence of 109° domain walls in the AC-poled samples, which contribute to more domain wall motion. These findings provide experimental evidence of collective domain wall motion and establish a direct connection between mesoscale dynamics and electromechanical response.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Exploring the scaling limitations of the variational quantum eigensolver with the bond dissociation of hydride diatomic molecules

Abstract Materials simulations involving strongly correlated electrons pose fundamental challenges to state‐of‐the‐art electronic structure methods but are hypothesized to be the ideal use case for quantum computing algorithms. To date, no quantum computer has simulated a molecule of a size and complexity relevant to real‐world applications, despite the fact that the variational quantum eigensolver (VQE) algorithm can predict chemically accurate total energies. Nevertheless, because of the many applications of moderately sized, strongly correlated systems, such as molecular catalysts, the successful use of the VQE stands as an important waypoint in the advancement toward useful chemical modeling on near‐term quantum processors. In this paper, we take a significant step in this direction. We lay out the steps, write, and run parallel code for an (emulated) quantum computer to compute the bond dissociation curves of the TiH, LiH, NaH, and KH diatomic hydride molecules using the VQE. TiH was chosen as a relatively simple chemical system that incorporates d orbitals and strong electron correlation. Because current VQE implementations on existing quantum hardware are limited by qubit error rates, the number of qubits available, and the allowable gate depth, recent studies using it have focused on chemical systems involving s and p block elements. Through VQE + UCCSD calculations of TiH, we evaluate the near‐term feasibility of modeling a molecule with d‐orbitals on real quantum hardware. We demonstrate that the inclusion of d‐orbitals and the use of the UCCSD ansatz, which are both necessary to capture the correct TiH physics, dramatically increase the cost of this problem. We estimate the approximate error rates necessary to model TiH on current quantum computing hardware using VQE + UCCSD and show them to likely be prohibitive until significant improvements in hardware and error correction algorithms are available.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Emerged Metallicity in Molecular Ferromagnetic Wires

Supramolecular engineering bridges molecular assembly with macromolecular charge-transfer salts, promising the design to construct supramolecular architectures that integrate cooperative properties difficult or impossible to find in conventional lattices. Here, we report the crystal engineering design and kinetic growth of one-dimensional supramolecular wires composed of bis(ethylenedithio)tetrathiafulvalene (ET + ) cation and polymeric Cu[N(CN) 2 ] 2 – anion. A bulk ferromagnetic order is discovered for filling up the gap where strong ferromagnetism is missing in such ET molecule-based charge-transfer salts. Metallicity is induced by electric current from the semiconducting wire, which is attributed to strain effect by tuning its close molecular contact. This structural feature is evidenced through the combination of various mechanistic spectroscopic studies. Further, electric dipole is established from the close molecular contacts and is suggestive to stabilize ferromagnetic spin interaction through anions bridging spin sites. The breakthrough shown here provides a pathway to explore low-dimensional supramolecular materials exhibiting strong electron correlation, metallicity, and ferromagnetism.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Emergence and manipulation of non-equilibrium Yu-Shiba-Rusinov states

The experimental advances in the study of time-dependent phenomena has opened a new path to investigating the complex electronic structure of strongly correlated and topological materials. Yu-Shiba-Rusinov (YSR) states induced by magnetic impurities in s-wave superconductors provide an ideal candidate system to study the response of a system to time-dependent manipulations of the magnetic environment. Here, we show that by imposing a time-dependent change in the magnetic exchange coupling, by changing the relative alignment of magnetic moments in an impurity dimer, or through a periodic drive of the impurity moment, one can tune the system through a time-dependent quantum phase transition, in which the system undergoes a transition from a singlet to a doublet ground state. We show that the electronic response of the system to external perturbations can be imaged through the time-dependent differential conductance, dI(t)/dV, which, in analogy to the equilibrium case, is proportional to a non-equilibrium local density of states. Our results open the path to visualizing the response of complex quantum systems to time-dependent external perturbations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump–probe experiments on condensed matter samples. Electron–phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron–phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. Here, we investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe 2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Dual-cone variational calculation of the two-electron reduced density matrix

The computation of strongly correlated quantum systems is challenging because of its potentially exponential scaling in the number of electron configurations. Variational calculation of the two-electron reduced density matrix (2-RDM) without the many-electron wave function exploits the pairwise nature of the electronic Coulomb interaction to compute a lower bound on the ground-state energy with polynomial computational scaling. Recently, a dual-cone formulation of the variational 2-RDM calculation was shown to generate the ground-state energy, albeit not the 2-RDM, at a substantially reduced computational cost, especially for higher $\textit{N}$-representability conditions such as the T2 constraint. Here we generalize the dual-cone variational 2-RDM method to compute not only the ground-state energy but also the 2-RDM. The central result is that we can compute the 2-RDM from a generalization of the Hellmann-Feynman theorem. Specifically, we prove that in the Lagrangian formulation of the dual-cone optimization the 2-RDM is the Lagrange multiplier. Further, we apply the method to computing the energies and properties of strongly correlated electrons—including atomic charges, electron densities, dipole moments, and orbital occupations—in an illustrative hydrogen chain and the nitrogen-fixation catalyst FeMoco. The dual variational computation of the 2-RDM with T2 or higher N -representability conditions provides a polynomially scaling approach to strongly correlated molecules and materials with significant applications in atomic and molecular and condensed-matter chemistry and physics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗