Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “self-consistent GW”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

51 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

An optimally tuned range-separated hybrid starting point for ab initio GW plus Bethe–Salpeter equation calculations of molecules

The ab initio GW plus Bethe–Salpeter equation (GW-BSE, where G is the one particle Green's function and W is the screened Coulomb interaction) approach has emerged as a leading method for predicting excitations in both solids and molecules with a predictive power contingent upon several factors. Among these factors are the (1) generalized Kohn–Sham eigensystem used to construct the GW self-energy and to solve the BSE and (2) the efficacy and suitability of the Tamm–Dancoff approximation. Here, we present a detailed benchmark study of low-lying singlet excitations from a generalized Kohn–Sham (gKS) starting point based on an optimally tuned range-separated hybrid (OTRSH) functional. We show that the use of this gKS starting point with one-shot G0W0 and G0W0-BSE leads to the lowest mean absolute errors (MAEs) and mean signed errors (MSEs), with respect to high-accuracy reference values, demonstrated in the literature thus far for the ionization potentials of the GW100 benchmark set and for low-lying neutral excitations of Thiel’s set molecules in the gas phase, without the need for self-consistency. The MSEs and MAEs of one-shot G0W0-BSE@OTRSH excitation energies are comparable to or lower than those obtained with other functional starting points after self-consistency. Additionally, we compare these results with linear-response time-dependent density functional theory (TDDFT) calculations and find GW-BSE to be superior to TDDFT when calculations are based on the same exchange-correlation functional. This work demonstrates tuned range-separated hybrids used in combination with GW and GW-BSE can greatly suppress starting point dependence for molecules, leading to accuracy similar to that for higher-order wavefunction-based theories for molecules without the need for costlier iterations to self-consistency.

McKeon, Caroline A. (ORCID:0000000217373503)↗
DOE OSTI2023

Gravitational Wave Eigenfrequencies from Neutrino-driven Core-collapse Supernovae

Abstract Core-collapse supernovae (CCSNe) are predicted to produce gravitational waves (GWs) that may be detectable by Advanced LIGO/Virgo. These GW signals carry information from the heart of these cataclysmic events, where matter reaches nuclear densities. Recent studies have shown that it may be possible to infer the properties of the proto-neutron star (PNS) via GWs generated by hydrodynamic perturbations of the PNS. However, we lack a comprehensive understanding of how these relationships may change with the properties of CCSNe. In this work, we build a self-consistent suite of over 1000 exploding CCSNe from a grid of progenitor masses and metallicities combined with six different nuclear equations of state (EOS). Performing a linear perturbation analysis on each model, we compute the resonant GW frequencies of the PNS, and we motivate a time-agnostic method for identifying characteristic frequencies of the dominant GW emission. From this, we identify two characteristic frequencies, of the early- and late-time signal, that measure the surface gravity of the cold remnant neutron star, and simultaneously constrain the hot nuclear EOS. However, we find that the details of the CCSN model, such as the treatment of gravity or the neutrino transport, and whether it explodes, noticeably change the magnitude and evolution of the PNS eigenfrequencies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Quasiparticle and Optical Properties of Carrier-Doped Monolayer MoTe 2 from First Principles

The intrinsic weak and highly nonlocal dielectric screening of two-dimensional materials is well-known to lead to high sensitivity of their optoelectronic properties to environment. Less studied theoretically is the role of free carriers in those properties. In this report we use ab initio GW and Bethe-Salpeter equation calculations, with a rigorous treatment of dynamical screening and local-field effects, to study the doping dependence of the quasiparticle and optical properties of a monolayer transition-metal dichalcogenide, 2H MoTe 2 . Here we predict a quasiparticle band gap renormalization of several hundreds of meV for experimentally attainable carrier densities and a similarly sizable decrease in the exciton binding energy. This results in an almost constant excitation energy for the lowest-energy exciton resonance with an increasing doping density. Using a newly developed and generally applicable plasmon-pole model and a self-consistent solution of the Bethe-Salpeter equation, we reveal the importance of accurately capturing both dynamical and local-field effects to understand detailed photoluminescence measurements.

2D material↗
DOE OSTI2021

Optical response and band structure of LiCoO 2 including electron-hole interaction effects

The optical response functions and band structures of LiCoO 2 are studied at different levels of approximation, from density functional theory (DFT) in the generalized gradient approximation (GGA) to quasiparticle self-consistent QSGW (with G for Green's function and W for screened Coulomb interaction) without and with ladder diagrams ($QSG\hat{W}$) and the Bethe Salpeter Equation (BSE) approach. The QSGW method is found to strongly overestimate the band gap and electron-hole or excitonic effects are found to be important. They lower the quasiparticle gap by only about 11~\% but the lowest energy peaks in absorption are found to be excitonic in nature. The contributions from different band to band transitions and the relation of excitons to band-to-band transitions are analyzed. Finally, the excitons are found to be strongly localized. Finally, a comparison to experimental data is presented.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Band gap renormalization, carrier mobilities, and the electron-phonon self-energy in crystalline naphthalene

Organic molecular crystals are expected to feature appreciable electron-phonon interactions that influence their electronic properties at zero and finite temperature. Here, we report first-principles calculations and an analysis of the electron-phonon self-energy in naphthalene crystals. We compute the zero-point renormalization and temperature dependence of the fundamental band gap, and the resulting scattering lifetimes of electronic states near the valence- and conduction-band edges employing density functional theory. Further, our calculated phonon renormalization of the GW-corrected quasiparticle band structure predicts a fundamental band gap of 5 eV for naphthalene at room temperature, in good agreement with experiments. From our calculated phonon-induced electron lifetimes, we obtain the temperature-dependent mobilities of electrons and holes in good agreement with experimental measurements at room temperature. Finally, we show that an approximate energy self-consistent computational scheme for the electron-phonon self-energy leads to the prediction of strong satellite bands in the electronic band structure. We find that a single calculation of the self-energy can reproduce the self-consistent results of the band gap renormalization and electrical mobilities for naphthalene, provided that the on-the-mass-shell approximation is used, i.e., if the self-energy is evaluated at the bare eigenvalues.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Stellar Mass Black Hole Formation and Multimessenger Signals from Three-dimensional Rotating Core-collapse Supernova Simulations

We present self-consistent 3D core-collapse supernova simulations of a 40 ${M}_{\odot }$ progenitor model using the isotropic diffusion source approximation for neutrino transport and an effective general relativistic potential up to `0.9 s postbounce. We consider three different rotational speeds with initial angular velocities of ${{\rm{\Omega }}}_{0}=0$, 0.5, and 1 rad s -1 and investigate the impact of rotation on shock dynamics, black hole (BH) formation, and gravitational wave (GW) signals. The rapidly rotating model undergoes an early explosion at ~250 ms postbounce and shows signs of the low $T/| W| $ instability. We do not find BH formation in this model within ~460 ms postbounce. In contrast, we find BH formation at 776 ms postbounce and 936 ms postbounce for the nonrotating and slowly rotating models, respectively. The slowly rotating model explodes at ~650 ms postbounce, and the subsequent fallback accretion onto the proto–neutron star (PNS) results in BH formation. In addition, the standing accretion shock instability induces rotation of the PNS in the model that started with a nonrotating progenitor. Assuming conservation of specific angular momentum during BH formation, this corresponds to a BH spin parameter of a = J/M = 0.046. However, if no explosion sets in, all the angular momentum will eventually be accreted by the BH, resulting in a nonspinning BH. The successful explosion of the slowly rotating model drastically slows down the accretion onto the PNS, allowing continued cooling and contraction that results in an extremely high GW frequency (f ~ 3000 Hz) at BH formation, while the nonrotating model generates GW signals similar to our corresponding 2D simulations.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Self-consistency in GWΓ formalism leading to quasiparticle-quasiparticle couplings

Within many-body perturbation theory, Hedin's formalism offers a systematic way to iteratively compute the self-energy Σ of any dynamically correlated interacting system, provided one can evaluate the interaction vertex Γ exactly. This is, however, impossible, in general, for it involves the functional derivative of Σ with respect to the Green's function. Here, we analyze the structure of this derivative, splitting it into four contributions and outlining the type of quasiparticle interactions that each of them generate. Moreover, we show how, in the implementation of self-consistency, the action of these contributions can be classified into two: A quantitative renormalization of previously included interaction terms and the inclusion of qualitatively distinct interaction terms through successive functional derivatives of Γ itself. Implementing this latter type of self-consistency can extend the validity of perturbative approximations based on Hedin's equations toward the high interaction limit, as we show in the example of the Hubbard dimer. Furthermore, our analysis also provides a unifying perspective on the perturbation theory landscape, showing how the T-matrix approach is completely contained in Hedin's formalism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Average nonlinear dynamics of particles in gravitational pulses: Effective Hamiltonian, secular acceleration, and gravitational susceptibility

Particles interacting with a prescribed quasimonochromatic gravitational wave (GW) exhibit secular (average) nonlinear dynamics that can be described by Hamilton’s equations. We derive the Hamiltonian of this “ponderomotive” dynamics to the second order in the GW amplitude for a general background metric. For the special case of vacuum GWs, we show that our Hamiltonian is equivalent to that of a free particle in an effective metric, which we calculate explicitly. We also show that already a linear GW pulse displaces a particle from its unperturbed trajectory by a finite distance that is independent of the GW phase and proportional to the integral of the pulse intensity.This effect is independent from the nonlinear memory effects that has been known. We calculate the particle displacement analytically and show that our result is in agreement with numerical simulations. We also show how the Hamiltonian of the nonlinear averaged dynamics naturally leads to the concept of the linear gravitational susceptibility of a particle gas with an arbitrary phase-space distribution. We calculate this susceptibility explicitly to apply it, in a follow-up paper, toward studying self-consistent GWs in inhomogeneous media within the geometrical-optics approximation

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Iterative subspace algorithms for finite-temperature solution of Dyson equation

One-particle Green’s functions obtained from the self-consistent solution of the Dyson equation can be employed in the evaluation of spectroscopic and thermodynamic properties for both molecules and solids. However, typical acceleration techniques used in the traditional quantum chemistry self-consistent algorithms cannot be easily deployed for the Green’s function methods because of a non-convex grand potential functional and a non-idempotent density matrix. Moreover, the optimization problem can become more challenging due to the inclusion of correlation effects, changing chemical potential, and fluctuations of the number of particles. In this paper, we study acceleration techniques to target the self-consistent solution of the Dyson equation directly. We use the direct inversion in the iterative subspace (DIIS), the least-squared commutator in the iterative subspace (LCIIS), and the Krylov space accelerated inexact Newton method (KAIN). We observe that the definition of the residual has a significant impact on the convergence of the iterative procedure. Based on the Dyson equation, we generalize the concept of the commutator residual used in DIIS and LCIIS and compare it with the difference residual used in DIIS and KAIN. The commutator residuals outperform the difference residuals for all considered molecular and solid systems within both GW and GF2. For a number of bond-breaking problems, we found that an easily obtained high-temperature solution with effectively suppressed correlations is a very effective starting point for reaching convergence of the problematic low-temperature solutions through a sequential reduction of temperature during calculations.

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

Study of self-interaction errors in density functional predictions of dipole polarizabilities and ionization energies of water clusters using Perdew-Zunger and locally scaled self-interaction corrected methods

Here, we studied the effects of self-interaction error (SIE) on the static dipole polarizabilities of water clusters modelled with three increasingly sophisticated, non-empirical density functional approximations (DFAs), viz. the local spin density approximation (LDA), the Perdew-Burke-Ernzherof (PBE) generalized-gradient approximation (GGA), and the strongly constrained and appropriately normed (SCAN) meta-GGA, using the Perdew-Zunger self-interaction-correction (PZ-SIC) energy functional in the Fermi-Lowdin orbital SIC (FLO-SIC) framework. Our results show that while all three DFAs overestimate the cluster polarizabilities, the description systematically improves from LDA to PBE to SCAN. The self-correlation free SCAN predicts polarizabilities quite accurately with a mean absolute error (MAE) of 0.58 Bohr 3 with respect to coupled cluster singles and doubles (CCSD) values. Removing SIE using PZ-SIC correctly reduces the DFA polarizabilities, but over-corrects, resulting in underestimated polarizabilities in SIC-LDA, -PBE, and -SCAN. Finally, we applied a recently proposed local-scaling SIC (LSIC) method using a quasi self-consistent scheme and using the kinetic energy density ratio as an iso-orbital indicator. The results show that the LSIC polarizabilities are in excellent agreement with mean absolute error of 0.08 Bohr 3 for LSIC-LDA and 0.06 Bohr 3 for LSIC-PBE with most recent CCSD polarizabilities. Likewise, the ionization energy estimates as an absolute of highest occupied energy eigenvalue predicted by LSIC are also in excellent agreement with CCSD(T) ionization energies with MAE of 0.4 eV for LSIC-LDA and 0.04 eV for LSIC-PBE. The LSIC-LDA predictions of ionization energies are comparable to the reported GW ionization energies while the LSIC-PBE ionization energies are more accurate than reported GW results.

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

GPAW: An open Python package for electronic structure calculations

We review the GPAW open-source Python package for electronic structure calculations. GPAW is based on the projector-augmented wave method and can solve the self-consistent density functional theory (DFT) equations using three different wave-function representations, namely real-space grids, plane waves, and numerical atomic orbitals. The three representations are complementary and mutually independent and can be connected by transformations via the real-space grid. This multi-basis feature renders GPAW highly versatile and unique among similar codes. By virtue of its modular structure, the GPAW code constitutes an ideal platform for the implementation of new features and methodologies. Moreover, it is well integrated with the Atomic Simulation Environment (ASE), providing a flexible and dynamic user interface. In addition to ground-state DFT calculations, GPAW supports many-body GW band structures, optical excitations from the Bethe–Salpeter Equation, variational calculations of excited states in molecules and solids via direct optimization, and real-time propagation of the Kohn–Sham equations within time-dependent DFT. A range of more advanced methods to describe magnetic excitations and non-collinear magnetism in solids are also now available. In addition, GPAW can calculate non-linear optical tensors of solids, charged crystal point defects, and much more. Recently, support for graphics processing unit (GPU) acceleration has been achieved with minor modifications to the GPAW code thanks to the CuPy library. We end the review with an outlook, describing some future plans for GPAW.

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

Improved quasiparticle self-consistent electronic band structure and excitons in β – LiGaO 2

The band structure of β–LiGaO 2 is calculated using the quasiparticle self-consistent QSGWˆ method where the screened Coulomb interaction Wˆ is evaluated including electron-hole interaction ladder diagrams and G is the one-electron Green's function. Improved convergence compared to previous calculations leads to a significantly larger band gap of about 7.0 eV. However, exciton binding energies are found to be large and lead to an exciton gap of about 6.0 eV if also a zero-point-motion correction of about –0.4 eV is included. Furthermore, these results are in excellent agreement with recent experimental results on the onset of absorption. Besides the excitons observed thus far, the calculations indicate the existence of a Rydberg-like series of exciton excited states, which is however modified from the classical Wannier exciton model by the anisotropies of the material and the more complex mixing of Bloch states in the excitons resulting from the Bethe-Salpeter equation. The exciton fine structure and the exciton wave functions are visualized and analyzed in various ways.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Slater transition methods for core-level electron binding energies

Methods for computing core-level ionization energies using self-consistent field (SCF) calculations are evaluated and benchmarked. These include a “full core hole” (or “ΔSCF”) approach that fully accounts for orbital relaxation upon ionization, but also methods based on Slater’s transition concept in which the binding energy is estimated from an orbital energy level that is obtained from a fractional-occupancy SCF calculation. A generalization that uses two different fractional-occupancy SCF calculations is also considered. The best of the Slater-type methods afford mean errors of 0.3–0.4 eV with respect to experiment for a dataset of K-shell ionization energies, a level of accuracy that is competitive with more expensive many-body techniques. An empirical shifting procedure with one adjustable parameter reduces the average error below 0.2 eV. Here, this shifted Slater transition method is a simple and practical way to compute core-level binding energies using only initial-state Kohn–Sham eigenvalues. It requires no more computational effort than ΔSCF and may be especially useful for simulating transient x-ray experiments where core-level spectroscopy is used to probe an excited electronic state, for which the ΔSCF approach requires a tedious state-by-state calculation of the spectrum. As an example, we use Slater-type methods to model x-ray emission spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Electronic structure and exchange interactions in altermagnetic MnGeP 2 in the quasiparticle self-consistent G W approach

The quasiparticle self-consistent 𝐺⁡𝑊 method is used to study the electronic band structure, optical dielectric function, and exchange interactions in chalcopyrite, 𝐼⁢ ‾ 4 ⁢2⁢𝑑, structure MnGeP 2 . The material is found to be an antiferromagnetic semiconductor with a lowest direct gap of 2.44 eV at the Γ point and a lower indirect gap of 1.87 eV from Γ to 𝑀. The material is an altermagnet because the two magnetic atoms of opposite spin are related by a twofold rotation operation perpendicular to the main fourfold rotation inversion axis. The spin splittings along a low symmetry line like 𝑃⁢𝑁 is sizable while at k points on the diagonal mirror planes or on the twofold symmetry axes the spin splitting is zero. The exchange interactions are calculated using a linear response approach. The antiferromagnetic exchange interaction between nearest neighbors in the primitive unit cell is dominating and found to be slightly decreasing upon carrier doping but not sufficiently to change the interaction to become ferromagnetic. The bare (noninteracting) and interacting transverse spin susceptibilities, which provide interatomic site exchange interactions after averaging over the muffin-tin spheres, are calculated from the 𝐺⁡𝑊 band structure and wave functions. From these exchange interactions, the spin wave spectra are obtained along the high symmetry lines and the Néel temperature is calculated using the mean-field and Tyablikov estimations. The dielectric function and the optical absorption spectra are calculated including excitonic effects using the Bethe Salpeter equation. The exchange interactions around Mn Ge defect sites is also studied. While we find it can generate ferromagnetic interactions with neighboring spins, we did not find direct evidence of producing an overall ferromagnetic phase. First, if Mn antisites are introduced by exchanging Mn with a nearby Ge, the interactions stay largely antiferromagnetic. Second, when we add additional Mn, in other words in Mn-rich stoichiometry, the Mn Ge antisites produce a strong ferromagnetic interaction primarily with the Mn in the same basal plane but weaker ferromagnetic interaction with adjacent plane Mn. The interactions between regular lattice Mn stay antiferromagnetic as before and thus favor keeping the antiferromagnetic order along the [001] direction. Adding Mn antisites, however, does lead to a metallic band structure.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Electron correlations in the cubic paramagnetic perovskite Sr ( V , Mn ) O 3 : Results from fully self-consistent self-energy embedding calculations

In this study, we use the thermodynamically consistent and conserving self-energy embedding theory (SEET) to study the spectra of the prototypical undistorted cubic perovskites SrVO 3 and SrMnO 3 . In the strongly correlated metallic SrVO 3 we find that the usual attribution of the satellite peaks at –1.8 eV to Hund or Hubbard physics in the t 2 g orbitals is inconsistent with our calculations. In the strongly correlated insulator SrMnO 3 we recover insulating behavior due to a feedback effect between the strongly correlated orbitals and the weakly correlated environment. Our calculation shows a systematic convergence of spectral features as the space of strongly correlated orbitals is enlarged, paving the way to a systematic parameter-free study of correlated perovskites.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗