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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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Topological phase transition to a hidden charge density wave liquid

Charge density waves (CDWs), electronic crystals that form within a host solid, have long been speculated to melt into a spatially textured electronic liquid. Though they have not been previously detected, liquid CDWs may nonetheless be fundamental to the phase diagrams of many correlated electron systems, including high temperature superconductors and quantum Hall states. In one of the most promising candidate materials capable of hosting a liquid CDW, 1T-TaS2, a structural phase transition impedes its observation. Here, by irradiating the material with a femtosecond light pulse, we circumvent the structural phase transition to reveal how topological defect dynamics govern the otherwise invisible CDW correlations. Upon photoexcitation, the CDW diffraction peaks broaden azimuthally, initially revealing a hexatic state. At higher temperatures, photoexcitation completely destroys translational and orientational order and only a ring of diffuse scattering is observed, a key signature of a liquid CDW. Our work provides compelling evidence for a defect-unbinding transition to a CDW liquid and presents a protocol for uncovering states that are hidden by other transitions in thermal equilibrium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Topological Excitations in Pyrochlore Heterostructures

This research project focuses on developing innovative materials that demonstrate unique quantum properties, specifically within electron systems that exhibit complex interactions, known as "correlated electron systems." Unlike non-correlated materials, finding topological phases (special states of matter with protected properties that make them stable against defects) in these correlated systems is a significant challenge. The project aims to design synthetic templates of two-dimensional "Kagome lattice" structures, made from specific materials called iridates and osmates, to study and control these exotic quantum behaviors. To achieve this, the project employs a cutting-edge spectroscopic tools that allow precise analysis of artificial quantum materials in terms of both energy and momentum while they are being created, using a specialized laser-based process called laser Molecular Beam Epitaxy.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Interplay of 𝑑- and 𝑝-states in RbTi3⁢Bi5 and CsTi3⁢Bi5 flat-band kagome metals

Shifting the Fermi level of the celebrated 𝐴⁢𝑀3⁢𝑋5 (135) compounds into proximity of flat bands strongly enhances electronic correlations and severely affects the formation of density waves and superconductivity. Our broadband infrared spectroscopy measurements of RbTi3⁢Bi5 and CsTi3⁢Bi5 combined with density-functional band-structure calculations reveal that the correlated Ti 𝑑-states are intricately coupled with the Bi 𝑝-states that form a tilted Dirac crossing. Electron-phonon coupling manifests itself in the strong damping of itinerant carriers and in the anomalous shape of the phonon line in RbTi3⁢Bi5. An anomaly in these spectral features around 150 K can be paralleled to the onset of nematicity detected by low-temperature probes. Our findings show that the materials with low band filling open unexplored directions in the physics of kagome metals and involve electronic states of different nature strongly coupled with lattice dynamics.

Wenzel, Matthew [ORNL]↗
DOE OSTI2021

Electronic structure of rhombohedral Cr X 3 ( X = Br, Cl, I) van der Waals crystals

We perform a comprehensive analysis of both the chemical and correlated electronic structure reconstruction of rhombohedral Cr X 3 (X = Br, Cl, I) van der Waals bulk crystals. Using the generalized gradient approximation (GGA) plus dynamical mean-field theory we explicitly demonstrate the importance of local dynamical correlations for a consistent understanding of emergent Kondo quasiparticles and Mott localized electronic states, showing the interplay between material-dependent one-electron GGA line-shape and multiorbital electronic interactions. To probe the correlated paramagnetic electronic state we performed x-ray absorption spectroscopy measurements for CrCl 3 and CrBr 3 bulk crystals. Furthermore, our correlated many-body study is relevant to understanding the electronic structure reconstruction of paramagnetic Cr-trihalide crystals and should be widely applicable to other van der Waals magnetic materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Emergent flat band electronic structure in a VSe 2 /Bi 2 Se 3 heterostructure

Flat band electronic states are proposed to be a fundamental tool to achieve various quantum states of matter at higher temperatures due to the enhanced electronic correlations. However, materials with such peculiar electronic states are rare and often rely on subtle properties of the band structures. Here, by using angle-resolved photoemission spectroscopy, we show the emergent flat band in a VSe 2 / Bi 2 Se 3 heterostructure. Our photoemission study demonstrates that the flat band covers the entire Brillouin zone and exhibits 2D nature with a complex circular dichroism. In addition, the Dirac cone of Bi 2 Se 3 is not reshaped by the flat band even though they overlap in proximity of the Dirac point. These features make this flat band distinguishable from the ones previously found. Thereby, the observation of a flat band in the VSe 2 / Bi 2 Se 3 heterostructure opens a promising pathway to realize strongly correlated quantum effects in topological materials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Observation of multiple flat bands and Van Hove singularities in the distorted kagome metal NdTi 3 Bi 4

Kagome materials have attracted enormous research interest recently owing to their diverse topological phases and manifestation of electronic correlation. Here, in this study, we present the electronic structure of a distorted ferromagnetic kagome metal, NdTi 3 ⁢Bi 4 , exhibiting a transition temperature of 9 K. Our investigation employs a combination of angle-resolved photoemission spectroscopy (ARPES) measurements and density functional theory (DFT) calculations. We discover the presence of two “flat” bands which are found to originate from the kagome structure formed by Ti atoms with a major contribution from Ti 𝑑 𝑥⁢𝑦 and Ti 𝑑 𝑥 2 −𝑦 2 orbitals. We also observed multiple Van Hove singularities (VHSs) in its electronic structure, with one VHS lying near the Fermi level. The ARPES data reveal the existence of Dirac cone at the $\overline{𝐾}$ point, a finding which is corroborated by our DFT calculations. These findings present a detailed electronic structure capable of hosting correlation-driven phenomenon in this novel ferromagnetic kagome metal.

Fermi surface↗
DOE OSTI2023

Magnetic Breakdown and Topology in the Kagome Superconductor CsV 3 Sb 5 under High Magnetic Field

The recently discovered layered kagome metals of composition AV 3 Sb 5 (A = K, Rb, Cs) exhibit a complex interplay among superconductivity, charge density wave order, topologically nontrivial electronic band structure and geometrical frustration. Here, we probe the electronic band structure underlying these exotic correlated electronic states in CsV 3 Sb 5 with quantum oscillation measurements in pulsed fields up to 86 T. The high-field data reveal a sequence of magnetic breakdown orbits that allows the construction of a model for the folded Fermi surface of CsV 3 Sb 5 . The dominant features are large triangular Fermi surface sheets that cover almost half the folded Brillouin zone. These sheets have not yet been detected in angle resolved photoemission spectroscopy and display pronounced nesting. In conclusion, the Berry phases of the electron orbits have been deduced from Landau level fan diagrams near the quantum limit without the need for extrapolations, thereby unambiguously establishing the nontrivial topological character of several electron bands in this kagome lattice superconductor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Discovery of charge density wave in a kagome lattice antiferromagnet

A hallmark of strongly correlated quantum materials is the rich phase diagram resulting from competing and intertwined phases with nearly degenerate ground state energies. A well-known example is the copper oxides, where a charge density wave (CDW) is ordered well above and strongly coupled to the magnetic order to form spin-charge separated stripes that compete with superconductivity. Recently, such rich phase diagrams have also been revealed in correlated topological materials. In two-dimensional kagome lattice metals consisting of corner-sharing triangles, the geometry of the lattice can produce flat bands with localized electrons, non-trivial topology, chiral magnetic order, superconductivity and CDW order. While CDW has been found in weakly electron correlated nonmagnetic AV 3 Sb 5 (A = K, Rb, Cs), it has not yet been observed in correlated magnetic ordered kagome lattice metals. Here we report the discovery of CDW within the antiferromagnetic (AFM) ordered phase of kagome lattice FeGe. The CDW in FeGe occurs at wavevectors identical to that of AV 3 Sb 5 , enhances the AFM ordered moment, and induces an emergent anomalous Hall effect. Furthermore, our findings suggest that CDW in FeGe arises from the combination of electron correlations-driven AFM order and van Hove singularities-driven instability possibly associated with a chiral flux phase, in stark contrast to strongly correlated copper oxides and nickelates, where the CDW precedes or accompanies the magnetic order.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Gutzwiller hybrid quantum-classical computing approach for correlated materials

Rapid progress in noisy intermediate-scale quantum (NISQ) computing technology has led to the development of novel resource-efficient hybrid quantum-classical algorithms, such as the variational quantum eigensolver (VQE), that can address open challenges in quantum chemistry, physics, and material science. Proof-of-principle quantum chemistry simulations for small molecules have been demonstrated on NISQ devices. While several approaches have been theoretically proposed for correlated materials, NISQ simulations of interacting periodic models on current quantum devices have not yet been demonstrated. Here, we develop a hybrid quantum-classical simulation framework for correlated electron systems based on the Gutzwiller variational embedding approach. We implement this framework on Rigetti quantum processing units (QPUs) and apply it to the periodic Anderson model, which describes a correlated heavy electron band hybridizing with noninteracting conduction electrons. Our simulation results quantitatively reproduce the known ground state quantum phase diagram including metallic, Kondo and Mott insulating phases. This is the first fully self-consistent hybrid quantum-classical simulation of an infinite correlated lattice model executed on QPUs, demonstrating that the Gutzwiller hybrid quantum-classical embedding framework is a powerful approach to simulate correlated materials on NISQ hardware. This benchmark study also puts forth a concrete pathway towards practical quantum advantage on NISQ devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Metallic support films reduce optical heating in cryogenic correlative light and electron tomography

Super-resolved cryogenic correlative light and electron tomography is an emerging method that provides both the single-molecule sensitivity and specificity of fluorescence imaging, and the molecular scale resolution and detailed cellular context of tomography, all in vitrified cells preserved in their native hydrated state. Technical hurdles that limit these correlative experiments need to be overcome for the full potential of this approach to be realized. Chief among these is sample heating due to optical excitation which leads to devitrification, a phase transition from amorphous to crystalline ice. Here, in this work, we show that much of this heating is due to the material properties of the support film of the electron microscopy grid, specifically the absorptivity and thermal conductivity. We demonstrate through experiment and simulation that the properties of the standard holey carbon electron microscopy grid lead to substantial heating under optical excitation. In order to avoid devitrification, optical excitation intensities must be kept orders of magnitude lower than the intensities commonly employed in room temperature super-resolution experiments. We further show that the use of metallic films, either holey gold grids, or custom made holey silver grids, alleviate much of this heating. For example, the holey silver grids permit 20× the optical intensities used on the standard holey carbon grids. Super-resolution correlative experiments conducted on holey silver grids under these increased optical excitation intensities have a corresponding increase in the rate of single-molecule fluorescence localizations. This results in an increased density of localizations and improved correlative imaging without deleterious effects from sample heating.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Multitude of topological phase transitions in bipartite dice and Lieb lattices with interacting electrons and Rashba coupling

We report the results of a Hartree-Fock study applied to interacting electrons moving in two different bipartite lattices: the dice and the Lieb lattices, at half-filling. Both lattices develop ferrimagnetic order in the phase diagram U-λ, where U is the Hubbard on-site repulsion and λ is the Rashba spin-orbit coupling strength. Our main result is the observation of an unexpected multitude of topological phases for both lattices. All these phases are ferrimagnetic, but they differ among themselves in their set of six Chern numbers (six numbers because the unit cells have three atoms). Here, the Chern numbers |C| observed in our study range from 0 to 3, showing that large Chern numbers can be obtained by the effect of electronic correlations, adding to the recently discussed methodologies to increase |C| based on extending the hopping range in tight-binding models, using sudden quenches, or photonic crystals, all without including electronic interactions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Sudden Collapse of Magnetic Order in Oxygen-Deficient Nickelate Films

Antiferromagnetic order is a common and robust ground state in the parent (undoped) phase of several strongly correlated electron systems. The progressive weakening of antiferromagnetic correlations upon doping paves the way for a variety of emergent many-electron phenomena including unconventional superconductivity, colossal magnetoresistance, and collective charge-spin-orbital ordering. In this study, we explored the use of oxygen stoichiometry as an alternative pathway to modify the coupled magnetic and electronic ground state in the family of rare earth nickelates ( RENiO 3 - x ). Using a combination of x-ray spectroscopy and resonant soft x-ray magnetic scattering, we find that, while oxygen vacancies rapidly alter the electronic configuration within the Ni and O orbital manifolds, antiferromagnetic order is remarkably robust to substantial levels of carrier doping, only to suddenly collapse beyond 0.21 e - / Ni without an accompanying structural transition. Our work demonstrates that ordered magnetism in RENiO 3 - x is mostly insensitive to carrier doping up to significant levels unseen in other transition-metal oxides. The sudden collapse of ordered magnetism upon oxygen removal may provide a new mechanism for solid-state magnetoionic switching and new applications in antiferromagnetic spintronics.

36 MATERIALS SCIENCE↗
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 OSTI2021

Ab initio study and assignment of electronic states in molecular RaCl

Radium compounds have attracted recently considerable attention due to both development of experimental techniques for high-precision laser spectroscopy of molecules with short-lived nuclei and amenability of certain radium compounds for direct cooling with lasers. Currently, radium monofluoride (RaF) is one of the most studied molecules among the radium compounds, both theoretically and recently also experimentally. Complementary studies of further diatomic radium derivatives are highly desired to assess the influence of chemical substitution on diverse molecular parameters, especially on those connected with laser cooling, such as vibronic transition probabilities, and those related to violations of fundamental symmetries. Here in this article high-precision ab initio studies of electronic and vibronic levels of diatomic radium monochloride (RaCl) are presented. Recently developed approaches for treating electronic correlation with Fock-space coupled cluster methods are applied for this purpose. Theoretical results are compared to an early experimental investigation by Lagerqvist and used to partially reassign the experimentally observed transitions and molecular electronic levels of RaCl. Effective constants of $\mathscr{P}$-odd hyperfine interaction W a and $\mathscr{P, T}$-odd scalar-pseudoscalar nucleus-electron interaction Ws in the ground electronic state of RaCl are estimated within the framework of a quasirelativistic Zeroth-Order Regular Approximation approach and compared to parameters in RaF and RaOH.

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

Angle-resolved nonresonant two-photon single ionization of argon using 9.3-eV photons produced via high-order harmonic generation

Here we present an experimental study on the photoionization dynamics of nonresonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3-eV photons produced via high harmonic generation and a three-dimensional momentum imaging spectrometer, we detect the photoelectrons and ions produced from nonresonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$- and $f$-partial-wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the vacuum ultraviolet polarization. The comparison between the present results and the two previous sets of theoretical calculations [Phys. Rev. A 44, 324 (1991), and J. Phys. B: At. Mol. Phys. 16, 2737 (1983)] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Orbital Ingredients and Persistent Dirac Surface State for the Topological Band Structure in FeTe 0.55 Se 0.45

FeTe 0.55 Se 0.45 (FTS) occupies a special spot in modern condensed matter physics at the intersections of electron correlation, topology, and unconventional superconductivity. The bulk electronic structure of FTS is predicted to be topologically nontrivial due to the band inversion between the d x z and p z bands along Γ − Z . However, there remain debates in both the authenticity of the Dirac surface states (DSSs) and the experimental deviations of band structure from the theoretical band inversion picture. Here we resolve these debates through a comprehensive angle-resolved photoemission spectroscopy investigation. We first observe a persistent DSS independent of k z . Then, by comparing FTS with FeSe, which has no band inversion along Γ − Z , we identify the spectral weight fingerprint of both the presence of the p z band and the inversion between the d x z and p z bands. Furthermore, we propose a renormalization scheme for the band structure under the framework of a tight-binding model preserving crystal symmetry. Our results highlight the significant influence of correlation on modifying the band structure and make a strong case for the existence of topological band structure in this unconventional superconductor. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗