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At least 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Ground and excited states of even-numbered Hubbard ring at half-filling: comparison of the extended Gutzwiller approach with exact diagonalization

It remains a great challenge in condensed matter physics to develop a method to treat strongly correlated many-body systems with balanced accuracy and efficiency. We introduce an extended Gutzwiller (EG) method incorporating a manifold technique, which builds an effective manifold of the many-body Hilbert space, to describe the ground- and excited-state properties of strongly correlated electrons. Here we systematically apply an EG projector onto the ground and excited states of a non-interacting system. Diagonalization of the true Hamiltonian within the manifold formed by the resulting EG wavefunctions gives the approximate ground and excited states of the correlated system. To validate this technique, we implement it on even-numbered fermionic Hubbard rings at half-filling with periodic boundary conditions, and compare the results with the exact diagonalization (ED) method. The EG method is capable of generating high-quality ground and low-lying excited state wavefunctions, as evidenced by the high overlaps of wavefunctions between the EG and ED methods. Favorable comparisons are also achieved for other quantities including the total energy, the double occupancy, the total spin and the staggered magnetization. With the capability of accessing the excited states, the EG method can capture the essential features of the one-electron removal spectral function that contains contributions from states deep in the excited spectrum. Finally, we provide an outlook on the application of this method on large extended systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Energy Frontier Research Centers: Center for the Computational Design of Functional Layered Materials (CCDM) August 1, 2014 - July 31, 2018; Center for Complex Materials from First Principles (CCM) August 1, 2018 - July 31, 2021 (Final Report)

The mission of the DOE Energy Frontier Research Centers CCDM (2014-2018) and CCM (2018-2021) was to theoretically develop, computationally apply, and experimentally validate electronic structure methods for all materials, with a focus on the complex materials, especially layered and two-dimensional materials, strongly-correlated materials, and liquid water. This was achieved by over 200 published journal articles authored by about 17 senior investigators from physics and chemistry and from theory, computation, and experiment, plus their collaborators. In particular, the Centers confirmed the predictive power of the SCAN (strongly constrained and appropriately normed) density functional, which was constructed to satisfy 17 known exact constraints and several appropriate norms. Without being fitted to real bonded systems, and at a modest computational cost, SCAN correctly predicted covalent, ionic, metallic, hydrogen, and van der Waals bonds in many challenging materials. SCAN gave an improved description of defects in semiconductors, surface properties of metals, seven phases of ice, liquid water, liquid and supercooled silicon, subtle structural distortions in ferroelectrics, formation energies and structural predictions for solids, and critical pressures for structural phase transitions. Perhaps most remarkably, SCAN correctly described some strongly-correlated materials that were previously believed to be beyond the reach of density-functional approximations. SCAN is the only density functional that correctly predicts the band gap closing under chemical doping of the cuprate high-temperature superconducting materials. SCAN also predicts a landscape of competing stripe and magnetic phases in the cuprates. For some materials with some codes, SCAN has convergence problems that are greatly reduced by the CCM-developed r 2 SCAN, without loss of accuracy or rigor. SCAN and r 2 SCAN still make some self-interaction error, which is greatly reduced by the CCDM/ CCM-developed local orbital scaling correction (LOSC). These Centers further proved that the fundamental energy gaps of a solid from an orbital energy difference and from total energy differences are the same for a large class of generalized Kohn-Sham (GKS) functionals, including SCAN and standard hybrid functionals, and that symmetry breaking arises when a dynamic density fluctuation drops to zero frequency. The Centers identified new mechanisms for catalysis in layered materials with ions intercalated between the layers, investigated charge density waves both in model systems and in real layered materials, studied changes of band gap with the number of layers, and explored topological ultrathin films, bent nanoribbons, and defects.

08 HYDROGEN↗
NASA NTRS2006

Pyroxenes in Martian meteorites as petrogenetic indicators

Pyroxenes in Martian meteorites are important recorders of petrogenetic processes. Understanding the details of pyroxene major and minor element compositional variations can provide important insights into those processes. A combination of careful petrographic analysis of natural samples and experimental crystallization studies can lead to better understanding of the processes that gave rise to these samples on Mars. In addition, experimentally determined major, minor and trace element partition coefficients are important for using natural pyroxenes to estimate the compositions of the melts from which they crystallized and the oxidation conditions that prevailed during crystallization. We will report on minor element (Al, Ti, Cr) zoning in nakhlite pyroxenes and in synthetic pyroxenes that we have grown for the purposes of determining pyroxene/melt partition coefficients for Sr and REE. The natural pyroxenes have patchy Al zoning that, by analogy with our experimental pyroxenes, we interpret as sector zoning. The irregular patchy nature of the zoning is probably the result of the vagaries of growth kinetics and local environment during crystal growth. More slowly cooled nakhlites have the most distinct bimodal zoning, with one mode having Al2O3 around 0.5-0.6 wt%, and the other around 0.9 %. Average Al content increases with increasing cooling rate. This feature is puzzling, since the cumulus pyroxenes were almost certainly present at the time of eruption. Al and Ti are strongly correlated, but Cr is completely decoupled from those elements. The synthetic pyroxenes are distinctly sector zoned in Al and Ti, and the sector-to-sector variation in Al within a single crystal has important effects on trace element partition coefficients. Trivalent REE are strongly correlated with Al, while divalent elements (Sr, Eu+2) show a significantly weaker correlation. For example, as the Al2O3 content varies from 0.3 to 0.6 wt % from one sector to another, D(Gd) increases by approx.80% while D(Sr) and D(Eu) only increase by 20-30% at oxygen fugacities near IW. The different Al dependency of D for trivalent REE vs. divalent Eu and Sr considerably complicates the calibration of the Eu oxybarometer.

McKay, Gordon↗
DOE OSTI2019

Spin-State Ordering in Metal-Based Compounds Using the Localized Active Space Self-Consistent Field Method

Quantitatively accurate calculations for spin-state ordering in transition-metal complexes typically demand a robust multiconfigurational treatment. The poor scaling of such methods with increasing size makes them impractical for large, strongly correlated systems. Density matrix embedding theory (DMET) is a fragmentation approach that can be used to specifically address this challenge. The single-determinantal bath framework of DMET is applicable in many situations, but it has been shown to perform poorly for molecules characterized by strong correlation when a multiconfigurational self-consistent field solver is used. To ameliorate this problem, the localized active space self-consistent field (LASSCF) method was recently described. Here in this work, LASSCF is applied to predict spin-state energetics in mono- and di-iron systems, and we show that the model offers an accuracy equivalent to that of CASSCF but at a substantially lower computational cost. Performance as a function of basis set and active space is also examined.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Neurointerventional Treatment in Acute Stroke. Whom to Treat? (Endovascular Treatment for Acute Stroke: Utility of THRIVE Score and HIAT Score for Patient Selection)

Purpose: Intra-arterial therapy (IAT) is used increasingly as a treatment option for acute stroke caused by central large vessel occlusions. Despite high rates of recanalization, the clinical outcome is highly variable. The authors evaluated the Houston IAT (HIAT) and the totaled health risks in vascular events (THRIVE) score, two predicting scores designed to identify patients likely to benefit from IAT. Methods: Fifty-two patients treated at the Stavanger University Hospital with IAT from May 2009 to June 2012 were included in this study. We combined the scores in an additional analysis. We also performed an additional analysis according to high age and evaluated the scores in respect of technical efficacy. Results: Fifty-two patients were evaluated by the THRIVE score and 51 by the HIAT score. We found a strong correlation between the level of predicted risk and the actual clinical outcome (THRIVE p = 0.002, HIAT p = 0.003). The correlations were limited to patients successfully recanalized and to patients <80 years. By combining the scores additional 14.3 % of the patients could be identified as poor candidates for IAT. Both scores were insufficient to identify patients with a good clinical outcome. Conclusions: Both scores showed a strong correlation to poor clinical outcome in patients <80 years. The specificity of the scores could be enhanced by combining them. Both scores were insufficient to identify patients with a good clinical outcome and showed no association to clinical outcome in patients aged {>=}80 years.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2012

Further Investigations of the Effect of Replacing Lithium by Sodium on Lithium Silicate Scintillating Glass Efficiency

Ce3+ doped lithium (6Li) silicate glasses are thermal neutron detectors. Prior work showed that when sodium (Na) is substituted for Li the scintillation efficiency, under beta particle stimulation, increased and then decreased as the sodium (Na) content was increased [1]. When all the 6Li was replaced by Na no scintillation was observed. Raman spectra, acquired using a visible excitation source provided no evidence of anomalous behavior. SEM microscopy did show some phase separation, but there was no obvious correlation with the scintillation efficiency. We have reexamined these glass samples using deep UV Raman excitation which reduces fluorescence interference. The newly acquired spectra show evidence of phase separation in the glasses. Specifically we see a peak at 800 cm-1 Raman shift which can be assigned to a vitreous silica moiety that results from phase separation. There is a strong correlation between this peak's area, the scintillation efficiency, and the Na content. The observed trend suggests that phase separation enhances scintillation and addition of Na reduces the amount of phase separation. We also see evidence of at least two defect structures that can be tentatively assigned to a three-membered ring structure and an oxygen vacancy. The latter is fairly strongly correlated with enhanced scintillation efficiency.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2011

The Crucial Role of Error Correlation for Uncertainty Modeling of CFD-Based Aerodynamics Increments

The Ares I ascent aerodynamics database for Design Cycle 3 (DAC-3) was built from wind-tunnel test results and CFD solutions. The wind tunnel results were used to build the baseline response surfaces for wind-tunnel Reynolds numbers at power-off conditions. The CFD solutions were used to build increments to account for Reynolds number effects. We calculate the validation errors for the primary CFD code results at wind tunnel Reynolds number power-off conditions and would like to be able to use those errors to predict the validation errors for the CFD increments. However, the validation errors are large compared to the increments. We suggest a way forward that is consistent with common practice in wind tunnel testing which is to assume that systematic errors in the measurement process and/or the environment will subtract out when increments are calculated, thus making increments more reliable with smaller uncertainty than absolute values of the aerodynamic coefficients. A similar practice has arisen for the use of CFD to generate aerodynamic database increments. The basis of this practice is the assumption of strong correlation of the systematic errors inherent in each of the results used to generate an increment. The assumption of strong correlation is the inferential link between the observed validation uncertainties at wind-tunnel Reynolds numbers and the uncertainties to be predicted for flight. In this paper, we suggest a way to estimate the correlation coefficient and demonstrate the approach using code-to-code differences that were obtained for quality control purposes during the Ares I CFD campaign. Finally, since we can expect the increments to be relatively small compared to the baseline response surface and to be typically of the order of the baseline uncertainty, we find that it is necessary to be able to show that the correlation coefficients are close to unity to avoid overinflating the overall database uncertainty with the addition of the increments.

Hemsch, Michael J.↗
DOE OSTI2017

Holography, Gravity and Condensed Matter

Over the five years of funding from this grant, I produced 26 publications. These include a book-long monograph on "Holographic Quantum Matter" that is currently in press with MIT press. The remainder were mostly published in Physical Review Letters, the Journal of High Energy Physics, Nature Physics, Classical and Quantum Gravity and Physical Review B. Over this period, the field of holography applied to condensed matter physics developed from a promising theoretical approach to a mature conceptual and practical edifice, whose ideas were realized in experiments. My own work played a central role in this development. In particular, in the final year of this grant, I co-authored two experimental papers in which ideas that I had developed in earlier years were shown to usefully describe transport in strongly correlated materials — these papers were published in Science and in the Proceedings of the National Academy of Sciences (obviously my contribution to these papers was theoretical). My theoretical work in this period developed several new directions of research that have proven to be influential. These include (i) The construction of highly inhomogeneous black hole event horizons, realizing disordered fixed points and describing new regimes of classical gravity, (ii) The conjecture of a bound on diffusivities that could underpin transport in strongly interacting media — an idea which may be proven in the near future and has turned out to be intimately connected to studies of quantum chaos in black holes and strongly correlated media, (iii) The characterization of new forms of hydrodynamic transport, e.g. with phase-disordered order parameters. These studies pertain to key open questions in our understanding of how non-quasiparticle, intrinsically strongly interacting systems can behave. In addition to the interface between holography and strongly interacting condensed matter systems, I made several advances on understanding the role of entanglement in quantum gravity. These included the first computation of holographic entanglement beyond the bulk classical limit as well understanding short distance entanglement in the emergent spacetime of the c=1 matrix quantum mechanics. The objective here is ultimately to understanding how a priori non-local degrees of freedom can re-arrange themselves quantum mechanically to support emergent local dynamics. Much of work funded by this grant involved collaboration with postdocs and graduate students, several of which were directly funded by the grant. These students have now successfully graduated to postdoctoral positions and in one case to high tech industry. The ideas developed in this work have directly fed into my current research in which I am aiming to prove fundamental bounds on entropy production and transport from quantum mechanics and statistical physics. As often, as with much of my previous work, black hole physics can be an inspiration for extreme dynamics such as fundamental bounds, but ultimately one hopes to prove them using more general tools of quantum field theory.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Magnesium, Iron and Aluminum in LLNL Air Particulate and Rain Samples with Reference to Magnesium in Industrial Storm Water

Storm water runoff from the Lawrence Livermore National Laboratory’s (LLNL’s) main site and Site 300 periodically exceeds the Discharge Permit Numeric Action Level (NAL) for Magnesium (Mg) under the Industrial General Permit (IGP) Order No. 2014-0057-DWQ. Of particular interest is the source of magnesium in storm water runoff from the site. This special study compares new metals data from air particulate and precipitation samples from the LLNL main site and Site 300 to previous metals data for storm water from the main site and Site 300 and alluvial sediment from the main site to investigate the potential source of elevated Mg in storm water runoff. Data for three metals (Mg, Iron {Fe}, and Aluminum {Al}) were available from all media; data for additional metals, such as Europium (Eu), were available from rain, air particulates, and alluvial sediment. To attribute source, this study compared metals concentration data (for Mg, Al, and Fe) in storm water and rain; metal-metal correlations (Mg with Fe, Mg with Al, Al with Fe, Mg with Eu, Eu with Fe, and Eu with Al) in storm water, rain, air particulates, and sediments; and metal-metal ratios ((Mg/Fe, Mg/Al, Al/Fe, Mg/Eu, Eu/Fe, and Eu/Al) in storm water, rain, air particulates and sediments. The results presented in this study are consistent with a simple conceptual model where the source of Mg in storm water runoff is air particulate matter that has dry-deposited on impervious surfaces and subsequently entrained in runoff during precipitation events. Such a conceptual model is consistent with 1) higher concentrations of metals in storm water runoff than in precipitation, 2) the strong correlation of Mg with Aluminum (Al) and Iron (Fe) in both storm water and air particulates, and 3) the similarity in metal mass ratios between storm water and air particulates in contrast to the dissimilarity of metal mass ratios between storm water and precipitation or alluvial sediment. The strong correlation of Mg with Fe and Al and of Fe with Al in storm water and air particulates and the strong association of Mg, Fe, and Al with Eu in air particulates strongly suggests that a dominant source of the Mg in storm water is associated with mineral phases of natural origin. These observations all point to Mg exceedances being associated with natural sources and processes and not with anthropogenic processes or pollutant sources.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Role of Surface Termination in the Metal–Insulator Transition of V 2 O 3 (0001) Ultrathin Films

Surface termination is known to play an important role in determining the physical properties of materials. It is crucial to know how surface termination affects the metal–insulator transition (MIT) of V 2 O 3 films for both fundamental understanding and its applications. By changing growth parameters, we achieved a variety of surface terminations in V 2 O 3 films that are characterized by low-energy electron diffraction (LEED) and photoemission spectroscopy techniques. Depending upon the terminations, our results show that MIT can be partially or fully suppressed near the surface region due to the different fillings of the electrons at the surface and subsurface layers and the change of screening length compared to the bulk. Across MIT, a strong redistribution of spectral weight and its transfer from a high-to-low-binding energy regime is observed in a wide energy scale. Our results show that the total spectral weight in the low-energy regime is not conserved across MIT, indicating a breakdown of the “sum rules of spectral weight”, signature of a strongly correlated system. Such a change in spectral weight is possibly linked to the change in hybridization, lattice volume (i.e., effective carrier density), and the spin degree of freedom in the system that occurs across MIT. We find that MIT in this system is strongly correlation-driven, where the electron–electron interactions play a pivotal role. Furthermore, our results provide better insight into the understanding of the electronic structure of strongly correlated systems and highlight the importance of accounting for surface effects during interpretation of the physical property data mainly using surface-sensitive probes, such as surface resistivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Exact PDF equations and closure approximations for advective-reactive transport

Mathematical models of advection–reaction phenomena rely on advective flow velocity and (bio) chemical reaction rates that are notoriously random. By using functional integral methods, we derive exact evolution equations for the probability density function (PDF) of the state variables of the advection–reaction system in the presence of random transport velocity and random reaction rates with rather arbitrary distributions. These PDF equations are solved analytically for transport with deterministic flow velocity and a linear reaction rate represented mathematically by a heterog eneous and strongly-correlated random field. Our analytical solution is then used to investigate the accuracy and robustness of the recently proposed large-eddy diffusivity (LED) closure approximation [1]. We find that the solution to the LED-based PDF equation, which is exact for uncorrelated reaction rates, is accurate even in the presence of strong correlations and it provides an upper bound of predictive uncertainty.

PDF methods, Uncertainty quantification, Heterogen↗
DOE OSTI2021

Visualizing electron localization of WS 2 /WSe 2 moiré superlattices in momentum space

The search for materials with flat electronic bands continues due to their potential to drive strong correlation and symmetry breaking orders. Electronic moirés formed in van der Waals heterostructures have proved to be an ideal platform. However, there is no holistic experimental picture for how superlattices modify electronic structure. By combining spatially resolved angle-resolved photoemission spectroscopy with optical spectroscopy, we report the first direct evidence of how strongly correlated phases evolve from a weakly interacting regime in a transition metal dichalcogenide superlattice. By comparing short and long wave vector moirés, we find that the electronic structure evolves into a highly localized regime with increasingly flat bands and renormalized effective mass. The flattening is accompanied by the opening of a large gap in the spectral function and splitting of the exciton peaks. These results advance our understanding of emerging phases in moiré superlattices and point to the importance of interlayer physics.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Coherent band excitations in CePd 3 : A comparison of neutron scattering and ab initio theory

In common with many strongly correlated electron systems, intermediate valence compounds are believed to display a crossover from a high-temperature regime of incoherently fluctuating local moments to a low-temperature regime of coherent hybridized bands. In this work, we show that inelastic neutron scattering measurements of the dynamic magnetic susceptibility of CePd 3 provides a benchmark for ab initio calculations based on dynamical mean field theory. The magnetic response is strongly momentum dependent thanks to the formation of coherent f-electron bands at low temperature, with an amplitude that is strongly enhanced by local particle-hole interactions. Finally, the agreement between experiment and theory shows that we have a robust first-principles understanding of the temperature dependence of f-electron coherence.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Fermi Gases in Bichromatic Superlattices

The purpose of the program is the broad study of designer materials made of ultra-cold atoms and light, which provides new paradigms for emulating exotic layered systems. Bichromatic superlattices enable control and study of both dimensionality and dispersion in layered, strongly correlated Fermi gases, to model high-temperature superfluidity/superconductivity. Most layered materials are quasi-two-dimensional, neither two-dimensional, like a sheet, nor three-dimensional, like a gas, but somewhere in between. In quasi-2D layers with an unequal number of spin-up and spin-down electrons, particularly strong attraction between pairs of electrons with opposite spins is predicted to achieve the highest possible superconducting transition temperatures. To understand these materials, we emulate them with a layered, ultra-cold Fermi gas of 6Li atoms, magnetically tuned near a collisional (Feshbach) resonance, where precise control of the attraction, spin-composition, dimensionality and dispersion provides new tests of theory. The primary goals are of the program are: (1) Elucidation of the effects of dimensionality and confining potential shape on the enhancement of high-temperature superfluidity in a layered, strongly correlated Fermi gases; (2) Control of dispersion and the study of tunable Dirac points in one dimension.

36 MATERIALS SCIENCE↗
DOE OSTI2012

MPS++

The MPS++ computer code simulates models of strongly correlated quantum lattice systems. The algorithm used is the density-matrix renormalization method formulated in the matrix product states language. These models and methods are used to obtain ground state, dynamic, finite temperature and time evolution properties of the underlying materials that are simulated. These materials are usually one- and quasi-one dimensional strongly correlated electronic systems, such as high temperature superconductors, manganites, and other transition metal oxides. This code is (mostly) an implementation of the paper “The density-matrix renormalization group in the age of matrix product states” by U. Schollwoeck, and references therein, found at http://arxiv.org/abs/1008.3477v2 , and that was also published in Annals of Physics 326,96 (2011).

Source record↗
DOE OSTI2012

MPS++

The MPS++ computer code simulates models of strongly correlated quantum lattice systems. The algorithm used is the density-matrix renormalization method formulated in the matrix product states language. These models and methods are used to obtain ground state, dynamic, finite temperature and time evolution properties of the underlying materials that are simulated. These materials are usually one- and quasi-one dimensional strongly correlated electronic systems, such as high temperature superconductors, manganites, and other transition metal oxides. This code is (mostly) an implementation of the paper "The density-matrix renormalization group in the age of matrix product states" by U. Schollwoeck, and references therein, found at http://arxiv.org/abs/1008.3477v2 , and that was also published in Annals of Physics 326,96 (2011).

Source record↗
DOE OSTI2017

Structural, electronic and magnetic properties of chevron-type graphene, BN and BC{sub 2}N nanoribbons

Graphene nanoribbons are predicted to be essential components in future nanoelectronics. The size, edge type, arrangement of atoms and width of nanoribbons drastically change their properties. Boronnitrogencarbon nanoribbons properties are not fully understood so far. In the present contribution it was investigated the structural, electronic and magnetic properties of chevron-type carbon, boron nitride and BC{sub 2}N nanoribbons, using first-principles calculations. The results indicate that the structural stability is closely related to the discrepancies in the bond lengths, which can induce structural deformations and stress. Such nanoribbons present a wide range of electronic behaviors, depending on their composition and particularities of the atomic arrangement. A net magnetic moment is found for structures that present carbon atoms at the nanoribbon borders. Nevertheless, the calculated magnetic moment depends on the peculiarities of the symmetric arrangement of atoms and imbalance of carbon atoms between different sublattices. It was found that all structures which have a significant energy gap do not present magnetic moment, and vice-versa. Such result indicates the strong correlation between the electronic and magnetic properties of the chevron-type nanoribbons. - Highlights: • Small discrepancies between distinct bond lengths can influence the formation energy of the BC{sub 2}N nanoribbons. • The electronic behavior of the BC{sub 2}N chevron-type nanoribbons depends on the atomic arrangement and structural symmetries. • There is a strong correlation between the electronic and magnetic properties for the BC{sub 2}N structures.

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

Crystal phases of charged interlayer excitons in van der Waals heterostructures

Throughout the years, strongly correlated coherent states of excitons have been the subject of intense theoretical and experimental studies. This topic has recently boomed due to new emerging quantum materials such as van der Waals (vdW) bound atomically thin layers of transition metal dichalcogenides (TMDs). We analyze the collective properties of charged interlayer excitons observed recently in bilayer TMD heterostructures. We predict strongly correlated phases—crystal and Wigner crystal—that can be selectively realized with TMD bilayers of properly chosen electron-hole effective masses by just varying their interlayer separation distance. Our results can be used for nonlinear coherent control, charge transport and spinoptronics application development with quantum vdW heterostuctures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗