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Results for “self-interaction correction”

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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72 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Photoelectron spectra of early 3 d -transition metal dioxide molecular anions from GW calculations

Photoelectron spectra of early 3 d -transition metal dioxide anions, Sc O 2 - , Ti O 2 - , V O 2 - , Cr O 2 - , and Mn O 2 - , are calculated using semilocal and hybrid density functional theory (DFT) and many-body perturbation theory within the GW approximation using one-shot perturbative and eigenvalue self-consistent formalisms. Different levels of theory are compared with each other and with available photoelectron spectra. We show that one-shot GW with a PBE0 starting point ( G 0 W 0 @PBE0) consistently provides very good agreement for all experimentally measured binding energies (within 0.1 eV–0.2 eV or less). We attribute this to the success of PBE0 in mitigating self-interaction error and providing good quasiparticle wave functions, which renders a first-order perturbative GW correction effective. One-shot GW calculations with a Perdew–Burke–Ernzerhof (PBE) starting point do poorly in predicting electron removal energies by underbinding orbitals with typical errors near 1.5 eV. A higher exact exchange amount of 50% in the DFT starting point of one-shot GW does not provide very good agreement with experiment by overbinding orbitals with typical errors near 0.5 eV. While not as accurate as G 0 W 0 @PBE0, the G -only eigenvalue self-consistent GW scheme with W fixed to the PBE level provides a reasonably predictive level of theory (typical errors near 0.3 eV) to describe photoelectron spectra of these 3 d -transition metal dioxide anions. Adding eigenvalue self-consistency also in W , on the other hand, worsens the agreement with experiment overall. Overall, our findings on the performance of various GW methods are discussed in the context of our previous studies on other transition metal oxide molecular systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1980

Gravitational radiation quadrupole formula is valid for gravitationally interacting systems

An argument is presented for the validity of the quadrupole formula for gravitational radiation energy loss in the far field of nearly Newtonian (e.g., binary stellar) systems. This argument differs from earlier ones in that it determines beforehand the formal accuracy of approximation required to describe gravitationally self-interacting systems, uses the corresponding approximate equation of motion explicitly, and evaluates the appropriate asymptotic quantities by matching along the correct space-time light cones.

Walker, M.↗
DOE OSTI2023

A tail of eternal inflation

Non-trivial inflaton self-interactions can yield calculable signatures of primordial non-Gaussianity that are measurable in cosmic surveys. We calculate the non-Gaussian corrections to Stochastic Inflation within the framework of Soft de Sitter Effective Theory, from which we derive the associated probability distribution for the scalar fluctuations. As a consequence of this new result, we show that the phase transition to slow-roll eternal inflation is often incalculable in these models. Instead, this transition is sensitive to the non-Gaussian tail of the distribution of scalar fluctuations, which probes physics inside the horizon, potentially beyond the cutoff scale of the Effective Field Theory of Inflation. We delineate the parameter space consistent with current observations and weak coupling at horizon crossing in which the large fluctuations relevant for eternal inflation can only be determined by appealing to a UV completion. We also argue that this breakdown of the perturbative description is required for the de Sitter entropy to reflect the number of de Sitter microstates.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Generating non-topological solitons via thermal corrections: Higgs balls

Scalar fields which carry charge can generally form non-topological solitons (Q-balls), if the energy in the extended configuration is less than the energy of an equivalent number of free quanta. For global Q-balls, such solitons exist whenever the potential grows slower than quadratically. We show that even in the absence of attractive interactions, finite temperature corrections can generate Q-ball solutions, as the coefficient of cubic corrections is generally negative. As an illustration of this, we consider the possibility of constructing Q-balls using the Higgs field. We first show that the finite temperature corrections would enable the existence of Higgs balls if the Standard Model symmetry was ungauged. We then consider gauged Q-balls, following [1], and demonstrate that Higgs self-interactions mediated by the Standard Model gauge bosons are sufficient to prevent the existence of these states in the actual Standard Model. However, these states can exist in a variety of extensions, as we show explicitly through an example.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Differential cross-section measurements of the production of four charged leptons in association with two jets using the ATLAS detector

Differential cross-sections are measured for the production of four charged leptons in association with two jets. These measurements are sensitive to final states in which the jets are produced via the strong interaction as well as to the purely-electroweak vector boson scattering process. The analysis is performed using proton-proton collision data collected by ATLAS at $\sqrt{s}$ = 13 TeV and with an integrated luminosity of 140 fb –1 . The data are corrected for the effects of detector inefficiency and resolution and are compared to state-of-the-art Monte Carlo event generator predictions. The differential cross-sections are used to search for anomalous weak-boson self-interactions that are induced by dimension-six and dimension-eight operators in Standard Model effective field theory.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Use of FLOSIC for understanding anion-solvent interactions

An Achille’s heel of lower-rung density-functional approximations is that the highest-occupied-molecular-orbital energy levels of anions, known to be stable or metastable in nature, are often found to be positive in the worst case or above the lowest-unoccupied-molecular-orbital levels on neighboring complexes that are not expected to accept charge. A trianionic example, [Cr(C2O4)3]3−, is of interest for constraining models linking Cr isotope ratios in rock samples to oxygen levels in Earth’s atmosphere over geological timescales. Here we describe how crowd sourcing can be used to carry out self-consistent Fermi–Löwdin–Orbital-Self-Interaction corrected calculations (FLOSIC) on this trianion in solution. The calculations give a physically correct description of the electronic structure of the trianion and water. In contrast, uncorrected local density approximation (LDA) calculations result in approximately half of the anion charge being transferred to the water bath due to the effects of self-interaction error. Use of group-theory and the intrinsic sparsity of the theory enables calculations roughly 125 times faster than our initial implementation in the large N limit reached here. By integrating charge density densities and Coulomb potentials over regions of space and analyzing core-level shifts of the Cr and O atoms as a function of position and functional, we unambiguously show that FLOSIC, relative to LDA, reverses incorrect solute-solvent charge transfer in the trianion-water complex. In comparison to other functionals investigated herein, including Hartree–Fock and the local density approximation, the FLOSIC Cr 1s eigenvalues provide the best agreement with experimental core ionization energies.

Chemistry↗
DOE OSTI2023

Loop corrections in Minkowski spacetime away from equilibrium. Part II. Finite-time results

Loop corrections to finite-time correlation functions in quantum field theories away from equilibrium can be calculated using the in-in path integral approach. In this paper, we calculate the unequal-time two-point correlator for different massless self-interacting scalar quantum field theories on a Minkowski background, starting the field evolution at an arbitrary initial time. We find the counterterms that need to be added to UV-renormalize the result, including usual in-out counterterms in the dynamics and additional initial state counterterms that are required to cancel all UV divergences. We find that the late-time limit of the renormalized correlation function exhibits a linear or logarithmic growth in time, depending on whether the interaction strength is dimension-one or dimensionless, respectively. The late-time correlations match those obtained in our companion paper and, as shown there, the divergences do not indicate a real IR issue, consistent with what one would expect in Minkowski.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Differential cross-section measurements for the electroweak production of dijets in association with a Z boson in proton–proton collisions at ATLAS

Differential cross-section measurements are presented for the electroweak production of two jets in association with a Z boson. These measurements are sensitive to the vector-boson fusion production mechanism and provide a fundamental test of the gauge structure of the Standard Model. The analysis is performed using proton–proton collision data collected by ATLAS at √s=13 TeV and with an integrated luminosity of 139 fb -1 . The differential cross-sections are measured in the Z→ℓ + ℓ - decay channel (ℓ=e,μ) as a function of four observables: the dijet invariant mass, the rapidity interval spanned by the two jets, the signed azimuthal angle between the two jets, and the transverse momentum of the dilepton pair. The data are corrected for the effects of detector inefficiency and resolution and are sufficiently precise to distinguish between different state-of-the-art theoretical predictions calculated using Powheg+Pythia8, Herwig7+Vbfnlo and Sherpa 2.2. The differential cross-sections are used to search for anomalous weak-boson self-interactions using a dimension-six effective field theory. The measurement of the signed azimuthal angle between the two jets is found to be particularly sensitive to the interference between the Standard Model and dimension-six scattering amplitudes and provides a direct test of charge-conjugation and parity invariance in the weak-boson self-interactions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Comparing GGA, GGA+ U , and meta-GGA functionals for redox-dependent binding at open metal sites in metal–organic frameworks

Metal–organic frameworks (MOFs) with open metal sites have been widely investigated for the selective adsorption of small molecules via redox mechanisms where charge transfer can take place between the binding site and the adsorbate of interest. Quantum-chemical screening methods based on density functional theory have emerged as a promising route to accelerate the discovery of MOFs with enhanced binding affinities toward various adsorbates. However, the success of this approach is linked to the accuracy of the underlying density functional approximations (DFAs). In this work, we compare commonly used generalized gradient approximation (GGA), GGA+U, and meta-GGA exchange-correlation functionals in modeling redox-dependent binding at open metal sites in MOFs using O 2 and N 2 as representative small molecules. We find that the self-interaction error inherent to the widely used Perdew, Burke, and Ernzerhof (PBE) GGA predicts metal sites that are artificially redox-active, as evidenced by their strong binding affinities, short metal–adsorbate bond distances, and large degree of charge transfer. The incorporation of metal-specific, empirical Hubbard U corrections based on the transition metal oxide literature systematically reduces the redox activity of the open metal sites, often improving agreement with experiment. Additionally, the binding behavior shifts from strong chemisorption to weaker physisorption as a function of U. The M06-L meta-GGA typically predicts binding energies between those of PBE-D3(BJ) and PBE-D3(BJ)+U when using empirically derived U values from the transition metal oxide literature. Despite the strong sensitivity of the binding affinities toward a given DFA, the GGA, GGA+U, and meta-GGA approaches often yield the same qualitative trends and structure–property relationships.

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

Nonequilibrium steady state and heat transport in nonlinear open quantum systems: Stochastic influence action and functional perturbative analysis

In this paper, we show that a nonequilibrium steady state (NESS) exists at late times in open quantum systems with weak nonlinearity by following its nonequilibrium dynamics with a perturbative analysis. We consider an oscillator chain containing three-types of anharmonicity: cubic α- and quartic β-type Fermi–Pasta–Ulam–Tsingou (FPUT) nearest-oscillator interactions and the on-site (pinned) Klein–Gordon (KG) quartic self-interaction. Assuming weak nonlinearity, we introduce a stochastic influence action approach to the problem and obtain the energy flows in different junctures across the chain. The formal results obtained here can be used for quantum transport problems in weakly nonlinear quantum systems. For α-type anharmonicity, we observe that the first-order corrections do not play any role in the thermal transport in the NESS of the configuration we considered. For KG and β-types anharmonicity, we work out explicitly the case of two weakly nonlinearly coupled oscillators, with results scalable to any number of oscillators. We examine the late-time energy flows from one thermal bath to the other via the coupled oscillators, and show that both the zeroth- and the first-order contributions of the energy flows become constant in time at late times, signaling the existence of a late-time NESS to first order in nonlinearity. Our perturbative calculations provide a measure of the strength of nonlinearity for nonlinear open quantum systems, which may help control the mesoscopic heat transport distinct from or close to linear transport. Furthermore, our results also give a benchmark for the numerical challenge of simulating heat transport. Our setup and predictions can be implemented and verified by investigating heat flow in an array of Josephson junctions in the limit of large Josephson energy with the platform of circuit QED.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1975

Comparison of theory and experiment for homogeneous turbulence with shear

Solutions for uniformly-sheared turbulence, in which the interaction of the turbulence with the mean shear dominates the turbulent self-interaction, are compared with experiment. An anisotropic spectral tensor, which appears general enough to represent the initial experimental turbulence, is used for the initial condition in the calculations. The evolution of one-point turbulence components and microscales, as well as two-point velocity correlations, are considered. In most cases the agreement with experiment is good. The theory correctly predicts the presence of a negative region for two-point longitudinal-velocity correlations only for point separations in the direction normal to the flow and the mean gradient.

Deissler, R. G.↗
DOE OSTI2020

Early-Universe Simulations of the Cosmological Axion

Ultracompact dark matter (DM) minihalos at masses at and below 10 –12 $M_⊙$ arise in axion DM models where the Peccei-Quinn (PQ) symmetry is broken after inflation. The minihalos arise from density perturbations that are generated from the nontrivial axion self-interactions during and shortly after the collapse of the axion-string and domain-wall network. We perform high-resolution simulations of this scenario starting at the epoch before the PQ phase transition and ending at matter-radiation equality. We characterize the spectrum of primordial perturbations that are generated and comment on implications for efforts to detect axion DM. In this work, we also measure the DM density at different simulated masses and argue that the correct DM density is obtained for $m_a$ = 25.2 ± 11.0 μ eV .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Measurements of W + W - + ≥ 1 jet production cross-sections in pp collisions at $ \sqrt{s} $ = 13 TeV with the ATLAS detector

Fiducial and differential cross-section measurements of W + W - production in association with at least one hadronic jet are presented. These measurements are sensitive to the properties of electroweak-boson self-interactions and provide a test of perturbative quantum chromodynamics and the electroweak theory. The analysis is performed using proton-proton collision data collected at $ \sqrt{s} $ = 13 TeV with the ATLAS experiment, corresponding to an integrated luminosity of 139 fb -1 . Events are selected with exactly one oppositely charged electron-muon pair and at least one hadronic jet with a transverse momentum of p T > 30 GeV and a pseudorapidity of |η| < 4.5. After subtracting the background contributions and correcting for detector effects, the jet-inclusive W + W - + ≥ 1 jet fiducial cross-section and W + W - + jets differential cross-sections with respect to several kinematic variables are measured. These measurements include leptonic quantities, such as the lepton transverse momenta and the transverse mass of the W + W - system, as well as jet-related observables such as the leading jet transverse momentum and the jet multiplicity. Limits on anomalous triple-gauge-boson couplings are obtained in a phase space where interference between the Standard Model amplitude and the anomalous amplitude is enhanced.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Delocalization error poisons the density-functional many-body expansion

The many-body expansion is a fragment-based approach to large-scale quantum chemistry that partitions a single monolithic calculation into manageable subsystems. This technique is increasingly being used as a basis for fitting classical force fields to electronic structure data, especially for water and aqueous ions, and for machine learning. Here, we show that the many-body expansion based on semilocal density functional theory affords wild oscillations and runaway error accumulation for ion–water interactions, typified by F − (H 2 O) N with N ≳ 15. We attribute these oscillations to self-interaction error in the density-functional approximation. The effect is minor or negligible in small water clusters, explaining why it has not been noticed previously, but grows to catastrophic proportion in clusters that are only moderately larger. This behavior can be counteracted with hybrid functionals but only if the fraction of exact exchange is ≳50%, whereas modern meta-generalized gradient approximations including ωB97X-V, SCAN, and SCAN0 are insufficient to eliminate divergent behavior. Other mitigation strategies including counterpoise correction, density correction (i.e., exchange–correlation functionals evaluated atop Hartree–Fock densities), and dielectric continuum boundary conditions do little to curtail the problematic oscillations. In contrast, energy-based screening to cull unimportant subsystems can successfully forestall divergent behavior. These results suggest that extreme caution is warranted when the many-body expansion is combined with density functional theory.

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

Comparative Density Functional Theory Study of Magnetic Exchange Couplings in Dinuclear Transition-Metal Complexes

Multicenter transition-metal complexes (MCTMs) with magnetically interacting ions have been proposed as components for information-processing devices and storage units. For any practical application of MCTMs as magnetic units, it is crucial to characterize their magnetic behavior, and in particular, the isotropic magnetic exchange coupling, J, between its magnetic centers. Due to the large size of typical MCTMs, density functional theory is the only practical electronic structure method for evaluating the J coupling. Here, we assess the accuracy of different density functional approximations for predicting the magnetic couplings of eight dinuclear transition-metal complexes, including five dimanganese, two dicopper, and one divanadium with known reliable experimental J couplings spanning from ferromagnetic to strong antiferromagnetic. The density functionals considered include global hybrid functionals which mix semilocal density functional approximations and exact exchange with a fixed admixing parameter, six local hybrid functionals where the admixing parameters are extended to be spatially dependent, the SCAN and r 2 SCAN meta-generalized gradient approximations (GGAs), and two widely used GGAs. We found that global hybrids tested in this work have a tendency to over-correct the error in magnetic coupling parameters from the Perdew–Burke–Ernzerhof (PBE) GGA as seen for manganese complexes. The performance of local hybrid density functionals shows no improvement in terms of bias and is scattered without a clear trend, suggesting that more efforts are needed for the extension from global to local hybrid density functionals for this particular property. The SCAN and r 2 SCAN meta-GGAs are found to perform as well as benchmark global hybrids on most tested complexes. We further analyze the charge density redistribution of meta-GGAs as well as global and local hybrid density functionals with respect to that of PBE, in connection to the self-interaction error or delocalization error.

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

Machine learning for accuracy in density functional approximations

Machine learning techniques have found their way into computational chemistry as indispensable tools to accelerate atomistic simulations and materials design. In addition, machine learning approaches hold the potential to boost the predictive power of computationally efficient electronic structure methods, such as density functional theory, to chemical accuracy and to correct for fundamental errors in density functional approaches. In this paper, recent progress in applying machine learning to improve the accuracy of density functional and related approximations is reviewed. Promises and challenges in devising machine learning models transferable between different chemistries and materials classes are discussed with the help of examples applying promising models to systems far outside their training sets.

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

Orbital dependent complications for close vs well-separated electrons in diradicals

We investigate two limits in open-shell diradical systems: O3, in which the interesting orbitals are in close proximity to one another, and (C21H13)2, where there is a significant spatial separation between the two orbitals. In accord with earlier calculations, we find that standard density-functional approximations do not predict the open-shell character for the former case but uniformly predict the open-shell character for the latter case. We trace the qualitatively incorrect behavior in O3 predicted by these standard density functional approximations to self-interaction error and use the Fermi–Löwdin-orbital-self-interaction-corrected formalism to determine accurate triplet, closed-shell singlet, and open-shell broken-spin-symmetry electronic configurations. Analysis of the resulting many-electron overlap matrices allows us to unambiguously show that the broken-spin-symmetry configurations do not participate in the representation of the Ms = 0 triplet states and allows us to reliably extract the singlet–triplet splitting in O3 by analyzing the energy as a function of Fermi-orbital-descriptor permutations. The results of these analyses predict the percentage of open-shell character in O3, which agrees well with conventional wavefunction-based methods. While these techniques are expected to be required in cases near the Coulson–Fischer point, we find that they will be less necessary in diradical systems with well-separated electrons, such as (C21H13)2. Results based on energies from self-interaction-corrected generalized gradient, local density, and Hartree–Fock approximations and experimental results are in generally good agreement for O3. These results help form the basis for deriving extended Heisenberg-like Hamiltonians that are needed for descriptions of molecular magnets when there are competing low-energy electronic configurations.

Chemistry↗
NASA NTRS2003

Computation of Large-Scale Structure Jet Noise Sources With Weak Nonlinear Effects Using Linear Euler

An approximate technique is presented for the prediction of the large-scale turbulent structure sound source in a supersonic jet. A linearized Euler equations code is used to solve for the flow disturbances within and near a jet with a given mean flow. Assuming a normal mode composition for the wave-like disturbances, the linear radial profiles are used in an integration of the Navier-Stokes equations. This results in a set of ordinary differential equations representing the weakly nonlinear self-interactions of the modes along with their interaction with the mean flow. Solutions are then used to correct the amplitude of the disturbances that represent the source of large-scale turbulent structure sound in the jet.

Dahl, Milo D.↗