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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Convergence and Quantum Advantage of Trotterized MERA for Strongly-Correlated Systems

Strongly-correlated quantum many-body systems are difficult to study and simulate classically. We recently proposed a variational quantum eigensolver (VQE) based on the multiscale entanglement renormalization ansatz (MERA) with tensors constrained to certain Trotter circuits. Here, we determine the scaling of computation costs for various critical spin chains which substantiates a polynomial quantum advantage in comparison to classical MERA simulations based on exact energy gradients or variational Monte Carlo. Algorithmic phase diagrams suggest an even greater separation for higher-dimensional systems. Hence, the Trotterized MERA VQE is a promising route for the efficient investigation of strongly-correlated quantum many-body systems on quantum computers. Furthermore, we show how the convergence can be substantially improved by building up the MERA layer by layer in the initialization stage and by scanning through the phase diagram during optimization. For the Trotter circuits being composed of single-qubit and two-qubit rotations, it is experimentally advantageous to have small rotation angles. We find that the average angle amplitude can be reduced considerably with negligible effect on the energy accuracy. Benchmark simulations suggest that the structure of the Trotter circuits for the TMERA tensors is not decisive; in particular, brick-wall circuits and parallel random-pair circuits yield very similar energy accuracies.

Miao, Qiang [Duke Quantum Center, Duke University,↗
DOE OSTI2022

Ultra-flat and long-lived plasmons in a strongly correlated oxide

Plasmons in strongly correlated systems are attracting considerable attention due to their unconventional behavior caused by electronic correlation effects. Recently, flat plasmons with nearly dispersionless frequency-wave vector relations have drawn significant interest because of their intriguing physical origin and promising applications. However, these flat plasmons exist primarily in low-dimensional materials with limited wave vector magnitudes (q< ~0.7 Å –1 ). Here, we show that long-lived flat plasmons can propagate up to ~1.2 Å –1 in α-Ti 2 O 3 , a strongly correlated three-dimensional Mott-insulator, with an ultra-small energy fluctuation (<40 meV). The strong correlation effect renormalizes the electronic bands near Fermi level with a small bandwidth, which is responsible for the flat plasmons in α-Ti 2 O 3 . Moreover, these flat plasmons are not affected by Landau damping over a wide range of wave vectors (q < ~1.2 Å –1 ) due to symmetry constrains on the electron wavefunctions. Our work provides a strategy for exploring flat plasmons in strongly correlated systems, which in turn may give rise to novel plasmonic devices in which flat and long-lived plasmons are desirable.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Importance of charge self-consistency in first-principles description of strongly correlated systems

First-principles approaches have been successful in solving many-body Hamiltonians for real materials to an extent when correlations are weak or moderate. As the electronic correlations become stronger often embedding methods based on first-principles approaches are used to better treat the correlations by solving a suitably chosen many-body Hamiltonian with a higher level theory. The success of such embedding theories, often referred to as second-principles, is commonly measured by the quality of self-energy Σ which is either a function of energy or momentum or both. However, Σ should, in principle, also modify the electronic eigenfunctions and thus change the real space charge distribution. While such practices are not prevalent, some works that use embedding techniques do take into account these effects. In such cases, choice of partitioning, of the parameters defining the correlated Hamiltonian, of double-counting corrections, and the adequacy of low-level Hamiltonian hosting the correlated subspace hinder a systematic and unambiguous understanding of such effects. Further, for a large variety of correlated systems, strong correlations are largely confined to the charge sector. Then an adequate nonlocal low-order theory is important, and the high-order local correlations embedding contributes become redundant. Here we study the impact of charge self-consistency within two example cases, TiSe 2 and CrBr 3 , and show how real space charge re-distribution due to correlation effects taken into account within a first-principles Green’s function-based many-body perturbative approach is key in driving qualitative changes to the final electronic structure of these materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A theory for colors of strongly correlated electronic systems

Many strongly correlated transition metal insulators are colored, even though they have band gaps much larger than the highest energy photons from the visible light. An adequate explanation for the color requires a theoretical approach able to compute subgap excitons in periodic crystals, reliably and without free parameters—a formidable challenge. The literature often fails to disentangle two important factors: what makes excitons form and what makes them optically bright. We pick two archetypal cases as examples: NiO with green color and MnF 2 with pink color, and employ two kinds of ab initio many body Green’s function theories; the first, a perturbative theory based on low-order extensions of the $GW$ approximation, is able to explain the color in NiO, while the same theory is unable to explain why MnF 2 is pink. We show its color originates from higher order spin-flip transitions that modify the optical response, which is contained in dynamical mean-field theory (DMFT). We show that symmetry lowering mechanisms may determine how ‘bright’ these excitons are, but they are not fundamental to their existence.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRSDate not supplied

Ab initio ground states of strongly-correlated materials on quantum computers

The accurate first-principles description of strongly-correlated materials is an important and challenging problem in condensed matter physics. Ab initio downfolding has emerged as a way of deriving accurate many-body Hamiltonians including strong correlations, representing a subspace of interest of a material, using density functional theory calculations as a starting point. However, the solution of these material-specific models can scale exponentially on classical computers, constituting a challenge. Here we propose that utilizing quantum computers for obtaining the properties of downfolded Hamiltonians yields an accurate description of the ground state properties of strongly-correlated systems, while circumventing the exponential scaling problem. We benchmark the solution of Hubbard-like models obtained through downfolding by utilizing a classical tensor network implementation of variational quantum eigensolvers (VQE), and we reveal a strategy for driving the optimization through a hybrid minimization of the energy and maximization of the overlap with an approximate solution obtained through low-cost computational methods. This results in a reduction of the energy error by orders of magnitude compared to conventional VQE approaches, and allows us to reproduce long-range correlations for the first time. We demonstrate our first-principles approach for diverse strongly-correlated materials, correctly predicting the antiferromagnetic state of one-dimensional cuprate Ca 2 CuO 3 , the excitonic ground state of monolayer WTe2, and the charge-ordered state of correlated metal SrVO 3 . Our efficient computational implementation allows us to simulate large systems with up to 54 qubits and encompassing up to four correlated bands, which is indicative of the complexity that our framework can address.

Antonios M Alvertis↗
DOE OSTI2026

Electronic transport, thermal transport, thermal expansion, and magnetization in the strongly correlated metal LaNi⁢O 3

Perovskite structured LaNiO 3 is a strongly correlated metal with intriguing thermal and magnetic properties. The volume dependence of calculated and measured physical properties can add additional critical information to develop a more in-depth understanding of this strongly correlated phenomenon. Taking advantage of recent single crystal LaNiO 3 growth using the floating-zone method, we have measured the thermal expansion, the magnetostriction, and the pressure dependence of the magnetic susceptibility, which then allows derivation of the Grüneisen parameters γ e = $\frac{dlnN(E_F)}{d lnV}$, γ χ = $\frac{dlnχ}{d lnV}$, as well as of electric and thermal transport properties. We simulate the volume dependence of structural and magnetic properties using Density Functional Theory calculations at the Generalized Gradient Approximation level. A large discrepancy between experimental values and calculated ones suggests that strong correlations are likely to be dynamic in nature. This study also provides a side-by-side comparison of measurements in single crystal and polycrystalline samples of LaNiO 3 to elucidate intrinsic materials properties. A broad hump at high temperatures in the temperature dependence of magnetization found in the single crystal sample of LaNiO 3 has been rationalized by a model that includes the influence of electron correlations on the Landau diamagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Active learning approach to simulations of strongly correlated matter with the ghost Gutzwiller approximation

Quantum embedding (QE) methods such as the ghost Gutzwiller approximation (gGA) offer a powerful approach to simulating strongly correlated systems, but come with the computational bottleneck of computing the ground state of an auxiliary embedding Hamiltonian (EH) iteratively. In this work, we introduce an active learning (AL) framework integrated within the gGA to address this challenge. The methodology is applied to the single-band Hubbard model and results in a significant reduction in the number of instances where the EH must be solved. Through a principal component analysis (PCA), we find that the EH parameters form a low-dimensional structure that is largely independent of the geometric specifics of the systems, especially in the strongly correlated regime. Our AL strategy enables us to discover this low-dimensionality structure on the fly, while leveraging it for reducing the computational cost of gGA, laying the groundwork for more efficient simulations of complex strongly correlated materials. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗
DOE OSTI2025

Compressing Hamiltonians with ab initio downfolding for simulating strongly-correlated materials on quantum computers

The accurate first-principles description of strongly correlated materials is an important and challenging problem in condensed matter physics. Ab initio downfolding has emerged as a way of deriving compressed many-body Hamiltonians that maintain the essential physics of strongly correlated materials. The solution of these material-specific models is still exponentially difficult to generate on classical computers, but quantum algorithms allow for a significant speed-up in obtaining the ground states of these compressed Hamiltonians. Here, we demonstrate that using quantum algorithms to obtain the properties of downfolded Hamiltonians can indeed yield high-fidelity solutions. By combining ab initio downfolding and variational quantum eigensolvers, we correctly predict the antiferromagnetic state of one-dimensional cuprate Ca 2 Cu O 3 , the excitonic ground state of monolayer W Te 2 , and the charge-ordered state of correlated metal Sr VO 3 . Numerical simulations using a classical tensor network implementation of variational quantum eigensolvers allow us to simulate large models with up to 54 qubits and encompassing up to four bands in the correlated subspace, which is indicative of the complexity that our framework can address. Through these methods we demonstrate the potential of classical preoptimization and downfolding techniques for enabling efficient materials simulation using quantum algorithms.

Alvertis, Antonios M. [NASA, Ames; LBNL, Berkeley]↗
DOE OSTI2022

Electronic structure of strongly correlated systems: recent developments in multiconfiguration pair-density functional theory and multiconfiguration nonclassical-energy functional theory

Strong electron correlation plays an important role in transition-metal and heavy-metal chemistry, magnetic molecules, bond breaking, biradicals, excited states, and many functional materials, but it provides a significant challenge for modern electronic structure theory. The treatment of strongly correlated systems usually requires a multireference method to adequately describe spin densities and near-degeneracy correlation. However, quantitative computation of dynamic correlation with multireference wave functions is often difficult or impractical. Multiconfiguration pair-density functional theory (MC-PDFT) provides a way to blend multiconfiguration wave function theory and density functional theory to quantitatively treat both near-degeneracy correlation and dynamic correlation in strongly correlated systems; it is more affordable than multireference perturbation theory, multireference configuration interaction, or multireference coupled cluster theory and more accurate for many properties than Kohn–Sham density functional theory. This perspective article provides a brief introduction to strongly correlated systems and previously reviewed progress on MC-PDFT followed by a discussion of several recent developments and applications of MC-PDFT and related methods, including localized-active-space MC-PDFT, generalized active-space MC-PDFT, density-matrix-renormalization-group MC-PDFT, hybrid MC-PDFT, multistate MC-PDFT, spin–orbit coupling, analytic gradients, and dipole moments. We also review the more recently introduced multiconfiguration nonclassical-energy functional theory (MC-NEFT), which is like MC-PDFT but allows for other ingredients in the nonclassical-energy functional. We discuss two new kinds of MC-NEFT methods, namely multiconfiguration density coherence functional theory and machine-learned functionals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Jordan–Wigner Transformation for the Description of Strong Correlation in Fermionic Systems

Seniority is a useful way of organizing Hilbert space for strongly correlated systems. The exact zero-seniority wave function, doubly occupied configuration interaction (DOCI), provides accurate results (given the right orbitals) for many strongly correlated electronic systems but has a combinatorial computational cost. In many cases, pair coupled cluster doubles provide a polynomial-cost approximation that closely reproduces the energies of DOCI, but it breaks down in some cases and, as shown herein, it does not provide particularly good density matrices. In this article, we demonstrate that by using the Jordan–Wigner transformation to turn the seniority zero problem back into a Fermionic one, we can provide mean-field variational results of DOCI quality for the Hubbard model and a few small molecular dissociation examples, with polynomial cost, both for the energies and for density matrices, all while being protected from collapse. This success is rooted in the proof we provide, showing that the Hartree–Fock wave function on the Jordan–Wigner-transformed Hamiltonian transforms back to variational coupled cluster doubles in the seniority zero representation, but restricted to have determinant rather than permanent amplitude coefficients, without compromising its overall accuracy.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Beyond quantum cluster theories: multiscale approaches for strongly correlated systems

The degrees of freedom that confer to strongly correlated systems their many intriguing properties also render them fairly intractable through typical perturbative treatments. For this reason, the mechanisms responsible for their technologically promising properties remain mostly elusive. Computational approaches have played a major role in efforts to fill this void. In particular, dynamical mean field theory and its cluster extension, the dynamical cluster approximation have allowed significant progress. However, despite all the insightful results of these embedding schemes, computational constraints, such as the minus sign problem in quantum Monte Carlo (QMC), and the exponential growth of the Hilbert space in exact diagonalization (ED) methods, still limit the length scale within which correlations can be treated exactly in the formalism. A recent advance aiming to overcome these difficulties is the development of multiscale many body approaches whereby this challenge is addressed by introducing an intermediate length scale between the short length scale where correlations are treated exactly using a cluster solver such QMC or ED, and the long length scale where correlations are treated in a mean field manner. At this intermediate length scale correlations can be treated perturbatively. This is the essence of multiscale many-body methods. Furthermore, we will review various implementations of these multiscale many-body approaches, the results they have produced, and the outstanding challenges that should be addressed for further advances.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Symmetry Breaking with the SCAN Density Functional Describes Strong Correlation in the Singlet Carbon Dimer

The SCAN (strongly constrained and appropriately normed) meta-generalized gradient approximation (meta-GGA), which satisfies all 17 exact constraints that a meta-GGA can satisfy, accurately describes equilibrium bonds that are normally correlated. With symmetry breaking, it also accurately describes some sd equilibrium bonds that are strongly correlated. While sp equilibrium bonds are nearly always normally correlated, the C 2 singlet ground state is known from correlated wave function theory to be a rare case of strong correlation in an sp equilibrium bond. Earlier work that calculated atomization energies of the molecular sequence B 2 , C 2 , O 2 , and F 2 in the local spin density approximation (LSDA), the Perdew–Burke–Ernzerhof (PBE) GGA, and the SCAN meta-GGA, without symmetry breaking in the molecule, found that only SCAN was accurate enough to reveal an anomalous under-binding for C 2 . Here, this work shows that spin symmetry breaking in singlet C 2 , which involves the appearance of net up- and down-spin densities on opposite sides (not ends) of the bond, corrects that underbinding, with a small SCAN atomization-energy error more like that of the other three molecules, suggesting that symmetry breaking with an advanced density functional might reliably describe strong correlation. This article also discusses some general aspects of symmetry breaking and the insights into strong correlation that symmetry breaking can bring. The normally correlated low-lying triplet excited state has the right vertical excitation energy in SCAN but not in LSDA or PBE, where the triplet is a false ground state. Fractional occupation numbers are found only for the symmetry-unbroken singlet and only in LSDA and PBE GGA.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Local lattice distortions and electronic orders in strongly correlated systems by resonant total x-ray scattering: A case study of A Pt 2 X 2 intermetallics ( A = U , Ce, or La and X = Si or Ge)

Revealing local lattice distortions in physical systems is nontrivial, largely because such structural features often are not necessarily amenable to traditional crystallographic investigations. This poses limits to our understanding of the underlying physic, particularly in the case of strongly correlated systems where structural, electronic and magnetic degrees of freedom are intertwined. Using resonant total x-ray scattering coupled to differential pair distribution function analysis, we reveal the presence of pronounced local lattice distortions in the square net Pt planes in the prototypical strongly correlated APt 2 X 2 intermetallics (A = U, Ce or La and X = Si or Ge). The distortions are present before charge density wave, magnetic, Kondo lattice coherence and/or superconducting orders emerge in these materials and, as density functional calculations suggest, are likely to affect them. Finally, our study sheds light on the poorly known interactions between electronic orders and structural disorder in strongly correlated systems and also demonstrates an advanced experimental approach to determine it that is relevant to any physical system showing deviations from perfect crystallinity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Transformer-based operator learning framework for self-energy in strongly correlated systems

We introduce Σ-Attention, a transformer-based operator-learning framework for approximating the self-energy operator of strongly correlated electronic systems. By creating a batched dataset that combines results from three complementary approaches, i.e., many-body perturbation theory, strong-coupling expansion, and exact diagonalization, each effective in specific parameter regimes, Σ-Attention is applied to learn an accurate approximation for the self-energy operator that is valid across a wide range of parameter regimes. This hybrid strategy leverages the strengths of existing methods while relying on the transformer's ability to generalize beyond individual limitations. More importantly, the scalability of the transformer architecture allows the learned self-energy to be extended to systems with larger sizes, leading to much improved computational scaling. Using the one-dimensional Hubbard model, we demonstrate that Σ-Attention can accurately predict the Matsubara Green's function of large systems with a wide range of coupling strength. Our framework offers a promising and scalable pathway for studying strongly correlated systems with many possible generalizations.

Zhu, Yuanran↗
DOE OSTI2025

Benchmarking Density Functional Theory Methods for Efficient Calculations of a Strongly Correlated Li 1– x Ni 1– y O 2−δ System

Transition metal oxides (TMOs), such as LiNiO 2 , are promising candidates for energy storage and electronic devices due to their unique electronic properties, exceptional physical and chemical characteristics, and ability to adopt multiple oxidation states. However, accurately predicting their properties using mean-field density functional theory (DFT) is challenging due to the presence of strongly correlated d-electrons and the complex interplay between their structural, electronic, and magnetic responses. These challenges are further exacerbated by the need to model defects, surfaces, and interfaces, which require computationally efficient, large-scale simulations. To address these issues, we carry out a benchmark study on the Li 1–x NiO 2 system, evaluating the performance of several popular functionals. Our findings demonstrate that combining SCAN functional relaxation with single-step HSE calculations provides a practical and scalable computational strategy. This approach balances accuracy and efficiency, enabling high-throughput simulations of strongly correlated TMOs and improved predictive modeling capability of TMOs for practical applications.

25 ENERGY STORAGE↗
DOE OSTI2024

Unravel Electronic Structure in Strongly Correlated Materials [Slides]

Outline: Introduction and motivation - Correlated electron materials; Theoretical approaches to strongly correlated materials - First-principles dynamical mean-field theory (DMFT) framework - Applications to f -electron correlation effects; Summary and outlook.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Strong-Weak Duality via Jordan-Wigner Transformation: Using Fermionic Methods for Strongly Correlated su(2) Spin Systems

The Jordan-Wigner transformation establishes a duality between $su(2)$ and fermionic algebras. We present qualitative arguments and numerical evidence that when mapping spins to fermions, the transformation makes strong correlation weaker, as demonstrated by the Hartree-Fock approximation to the transformed Hamiltonian. This result can be rationalized in terms of rank reduction of spin shift terms when transformed to fermions. Conversely, the mapping of fermions to qubits makes strong correlation stronger, complicating its solution when one uses qubit-based correlators. The presence of string operators poses challenges to the implementation of quantum chemistry methods on classical computers, but these can be dealt with using established techniques of low computational cost. Here, our proof of principle results for XXZ and J1-J2 Heisenberg (in 1D and 2D) indicate that the JW transformed fermionic Hamiltonian has reduced complexity in key regions of their phase diagrams, and provides a better starting point for addressing challenging spin problems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Mutual information prediction for strongly correlated systems

We have trained a new machine-learning (ML) model which predicts mutual information (MI) for strongly correlated systems. This is a complex quantity, which is much more difficult to predict than one-site entropies, but carries important information about the correlation structure inside electronic systems. In this work, we replaced the expensive density matrix renormalization group (DMRG) calculations by newly trained ML model for prediction of the mutual information. We show the performance of the model on two important tasks: (a) to determine the correlation structure and (b) to determine ordering of orbitals for accurate DMRG calculations. In conclusion, the results are compared with the MI obtained from accurate DMRG calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗