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Results for “time-dependent 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.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Giant self-driven exciton-Floquet signatures in time-resolved photoemission spectroscopy of MoS 2 from time-dependent GW approach

Time-resolved, angle-resolved photoemission spectroscopy (TR-ARPES) is a one-particle spectroscopic technique that can probe excitons (two-particle excitations) in momentum space. We present an ab initio, time-domain GW approach to TR-ARPES and apply it to monolayer MoS 2 . We show that photoexcited excitons may be measured and quantified as satellite bands and lead to the renormalization of the quasiparticle bands. These features are explained in terms of an exciton-Floquet phenomenon induced by an exciton time–dependent bosonic field, which are orders of magnitude stronger than those of laser field–induced Floquet bands in low-dimensional semiconductors. Our findings imply a way to engineer Floquet matter through the coherent oscillation of excitons and open the new door for mechanisms for band structure engineering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Light-induced shift current vortex crystals in moiré heterobilayers

Transition metal dichalcogenide (TMD) moiré superlattices provide an emerging platform to explore various light-induced phenomena. Recently, the discoveries of novel moiré excitons have attracted great interest. The nonlinear optical responses of these systems are however still underexplored. Here, we report investigation of light-induced shift currents (a second-order response generating DC current from optical illumination) in the WSe 2 /WS 2 moiré superlattice. We identify a striking phenomenon of the formation of shift current vortex crystals—i.e., two-dimensional periodic arrays of moiré-scale current vortices and associated magnetic fields with remarkable intensity under laboratory laser setup. Furthermore, we demonstrate high optical tunability of these current vortices—their location, shape, chirality, and magnitude can be tuned by the frequency, polarization, and intensity of the incident light. Electron-hole interactions (excitonic effects) are found to play a crucial role in the generation and nature of the shift current intensity and distribution. Our findings provide a promising all-optical control route to manipulate nanoscale shift current density distributions and magnetic field patterns, as well as shed light on nonlinear optical responses in moiré quantum matter and their possible applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Excitonic Interactions and Mechanism for Ultrafast Interlayer Photoexcited Response in van der Waals Heterostructures

Optical dynamics in van der Waals heterobilayers is of fundamental scientific and practical interest. Based on a time-dependent adiabatic GW approach, we discover a new many-electron (excitonic) channel for converting photoexcited intralayer to interlayer excitations and the associated ultrafast optical responses in heterobilayers, which is conceptually different from the conventional single-particle picture. We find strong electron-hole interactions drive the dynamics and enhance the pump-probe optical responses by an order of magnitude with a rise time of ~3⁢0⁢0 fs in MoSe 2 /WSe 2 heterobilayers, in agreement with experiment.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Electronic structure and optical properties of halide double perovskites from a Wannier-localized optimally-tuned screened range-separated hybrid functional

Halide double perovskites are a chemically diverse and growing class of compound semiconductors that are promising for optoelectronic applications. However, the prediction of their fundamental gaps and optical properties with density functional theory (DFT) and ab initio many-body perturbation theory has been a significant challenge. Recently, a nonempirical Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional has been shown to accurately produce the fundamental band gaps of a wide set of semiconductors and insulators, including lead halide perovskites. Here, in this study, we apply the WOT-SRSH functional to five halide double perovskites and compare the results with those obtained from other known functionals and previous GW calculations. We also use the approach as a starting point for GW calculations and we compute the band structures and optical absorption spectrum for Cs 2 AgBiBr 6 , using both time-dependent DFT and the GW-Bethe-Salpeter equation approach. We show that the WOT-SRSH functional leads to accurate fundamental and optical band gaps, as well as optical absorption spectra, consistent with spectroscopic measurements, thereby establishing WOT-SRSH as a viable method for the accurate prediction of optoelectronic properties of halide double perovskites.

36 MATERIALS SCIENCE↗
NASA NTRS1992

The Great Wall in the CfA survey - Its origin and imprint on the microwave background radiation

The paper models the evolution of the Great Wall (GW) after recombination and the influence of its time-dependent gravitational potential on the MBR. It is shown that within the framework of the Zel'dovich approximation the (pre)GW region can be treated as an ellipsoid. The GW is approximated as an oblate ellipsoid that started at recombination with an almost spherical shape, but with initial density contrast, delta-i, much smaller than it had to be in the spherical model in order to reach the observed density contrast of beta-f of 5. The resultant delta-i is compatible with the rms value of delta-rho/rho on the GW scale at recombination for models with the n less than 0 power spectrum of the primordial density field. It is shown that the time-dependent potential of the GW will induce a detectable fluctuation in MBR. The possibility of similar structures located at higher redshifts producing measurable and perhaps dominant statistical MBR anisotropies by this effect is also discussed.

Atrio-Barandela, F.↗
DOE OSTI2024

Time-dependent density functional theory with the orthogonal projector augmented wave method

The projector augmented wave (PAW) method of Blöchl linearly maps smooth pseudo wavefunctions to the highly oscillatory all-electron DFT orbitals. Compared to norm-conserving pseudopotentials (NCPP), PAW has the advantage of lower kinetic energy cutoffs and larger grid spacing at the cost of having to solve for non-orthogonal wavefunctions. We earlier developed orthogonal PAW (OPAW) to allow the use of PAW when orthogonal wavefunctions are required. In OPAW, the pseudo wavefunctions are transformed through the efficient application of powers of the PAW overlap operator with essentially no extra cost compared to NCPP methods. Previously, we applied OPAW to DFT. Here, we take the first step to make OPAW viable for post-DFT methods by implementing it in real-time time-dependent (TD) DFT. Using fourth-order Runge–Kutta for the time-propagation, we compare calculations of absorption spectra for various organic and biological molecules and show that very large grid spacings are sufficient, 0.6–0.7 bohr in OPAW-TDDFT rather than the 0.4–0.5 bohr used in traditional NCPP-TDDFT calculations. This reduces the memory and propagation costs by around a factor of 3. Our method would be directly applicable to any post-DFT methods that require time-dependent propagations such as the GW approximation and the Bethe–Salpeter equation.

Chemistry↗
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 OSTI2021

Kohn-Sham Solver (KSSOLV) v2.0

KSSOLV is a MATLAB toolbox for solving Kohn-Sham density functional theory based electronic structure eigenvalue problems. It uses an object oriented features of MATLAB to represent atom, molecules, wavefunctions and Hamiltonians and their operations. It is designed to make it easier for users to prototype and test new algorithms for solving the Kohn-Sham problem. KSSOLV2.0 contains significant improvement over the original KSSOLV described in a paper published in ACM Transaction on Mathematical Software (attached). In addition to performing ground state calculation for small molecules, it can also perform geometry optimization for both molecules and solids. It uses standard pseudopotentials and implements local density approximation, generalized gradient approximation and hybrid functionals. Future releases will also include time-dependent DFT and post DFT calculations such as the GW quasi-particle energy calculation and Bethe-Salpeter equation solver for optical absorption.

Yang, Chao↗
DOE OSTI2024

GW with hybrid functionals for large molecular systems

A low-cost approach for stochastically sampling static exchange during time-dependent Hartree–Fock-type propagation is presented. This enables the use of an excellent hybrid density functional theory (DFT) starting point for stochastic GW quasiparticle energy calculations. Generalized Kohn–Sham molecular orbitals and energies, rather than those of a local-DFT calculation, are used for building the Green function and effective Coulomb interaction. The use of an optimally tuned hybrid diminishes the starting point dependency in one-shot stochastic GW, effectively avoiding the need for self-consistent GW iterations.

Chemistry↗
DOE OSTI2026

Time-dependent scenario modeling for the ST-E1 fusion power plant

ST-E1 is a low aspect ratio fusion power plant being designed by Tokamak Energy targeting 1.5 GW of fusion power. Characterization of the ST-E1 flat-top scenario is described elsewhere McNamara et al (2026 Nucl. Fusion 66 086008); here we focus on addressing the question of how to ramp-up the ST-E1 plasma from an initial state following breakdown and flux-surface formation to the target flat-top state. Being low-aspect ratio, the available solenoid flux of ST-E1 is limited. Therefore, particular consideration is placed on developing ramp-up scenarios that predominantly use inductive flux provided by external vertical field coils. Through time-dependent modeling with METIS, we show that this is possible when the ramp-up is performed at relatively high plasma density: although auxiliary current drive efficiency is reduced, this is significantly outweighed by (1) higher electron-ion collisional equilibration, (2) higher fusion power once ions become sufficiently hot, (3) higher poloidal beta for increased vertical-field flux, and (4) potentially favorable exhaust compatibilities. Ultimately, we show the target ST-E1 flat-top performance can be reached after a ramp-up period lasting 150 s using less than 40 Vs of solenoid flux (with vertical field providing ∼ 90 Vs of flux). The sensitivity to model assumptions are presented, with the general observation that deleterious effects can be mitigated through minor alterations of the auxiliary power temporal waveform and/or total auxiliary power level. The impact of a solenoid and the auxiliary power mix (electron cyclotron heating only versus electron and ion cyclotron heating) on the ST-E1 ramp-up success are also discussed in appendices. On this latter topic, we show that the effect of direct-ion heating during ramp-up is obscured by the uncertainty in the pedestal dynamics, identifying a clear line of future work required to make a definite decision on the ST-E1 auxiliary power mix.

current ramp-up↗
DOE OSTI2024

Optoelectronic properties of bent two-dimensional materials from first-principles methods combined with machine learning

A material’s interaction with light is highly relevant in the design of nanoelectronic devices such as photodiodes, solar cells, photocatalytic cells, phototransistors, and photodetectors. The interaction of a material with light can be altered by mechanical deformation. Fine tuning of the optical properties can be achieved by mechanical bending that alters the electronic structure. Optical properties strongly depend on band gaps, therefore any alteration in the band structure results in a changed optical response of the material. The impact of bending was explored in this project. The goal of this project was to assess the impact of mechanical bending of two-dimensional transition metal dichalcogenides on their optoelectronic properties, using first-principles methods. These first-principles approximations are largely built upon many-body theory for the optical properties of magnetic and topological nanoribbons. GW-BSE is standard for optical absorption, but it is less practical for collective excitations as it was shown in model systems. Time-dependent density functional theory, however, has better promises for collective excitations in low-dimensional materials.

36 MATERIALS SCIENCE↗
NASA NTRS2000

Modeling the Dynamics of the Middle Atmosphere and Lower Thermosphere Under the Influence of Gravity Waves

Our Numerical Spectral Model (NSM), which extends from the ground up into the thermosphere, is non-linear, time-dependent and has been employed for 2D and 3D applications. The standard version of the NSM incorporates Hines' Doppler Spread Parameterization for small scale gravity waves (GW), but planetary waves generated in the troposphere have also been incorporated. The NSM has been applied to describe: (1) the anomalous seasonal variations of the zonal circulation and temperature in the upper mesosphere, (2) the equatorial oscillations (quasi-biennial and semi-annual oscillations (QBO and SAO)) extending from the stratosphere into the upper mesosphere, (3) the diurnal and semi-diurnal tides, and (4) the planetary waves that are excited in the mesosphere. With the emphasis to provide understanding, we present here results from numerical experiments with the NSM that shed light on the GW processes that are of central importance in the mesosphere and lower thermosphere. These are our conclusions: (1) The large semiannual variations in the diurnal tide (DT), with peak amplitudes observed around equinox, are produced primarily by GW interactions that involve, in part, planetary waves. The DT, like planetary waves, tends to be amplified by GW momentum deposition, which reduces also the vertical wavelength, but variations in eddy viscosity associated with GW interactions are also important. (2) The semidiurnal tide (SDT) and its phase in particular, is strongly influenced by the mean zonal circulation. The SDT, individually, is also amplified by GW. But the DT filters out GW such that the GW interaction effectively reduces the amplitude of the SDT, producing a strong nonlinear interaction between the DT and SDT. (3) Without external time dependent energy or momentum sources, planetary waves (PW) are generated in the model for zonal wavenumbers 1 to 4, which have amplitudes in the mesosphere above 50 km as large as 40 m/s and periods between 50 and 2 days. The waves are generated primarily during solstice conditions, which indicates that the baroclinic instability (associated with the GW induced reversal in the latitudinal temperature gradient) is playing an important role. Numerical experiment show that GW, directly, also greatly amplify the PW. A common feature of the PW generated in summer and winter is that their vertical wavelengths throughout the mesosphere are large, which indicates that the waves are not propagating freely but are generated throughout the region. Another common feature is that the PW propagate preferentially westward in summer and eastward in winter, being launched from the westward and eastward zonal winds that prevail respectively in summer and winter at altitudes below 80 km. (4) Planetary waves generated internally by baroclinic instability and GW interaction produce large amplitude modulations of the DT and SDT. In summary we conclude that GW play major roles in generating and amplifying the dynamical components in the MLT region and, acting principally through wave filtering, produce important non-linear interactions between the components.

Mayr, H. G.↗
DOE OSTI2021

Theory of Plasmonic Hot-Carrier Generation and Relaxation

Hot-carrier (HC) generation from (localized) surface plasmon decay has recently attracted much attention due to its promising applications in physical, chemical, materials, and energy science. However, the detailed mechanisms of plasmonic HC generation, relaxation, and trapping are less studied. In this work, we developed and applied a quantum-mechanical model and coupled master equation method to study the generation of HCs from plasmon decay and their following relaxation processes with different mechanisms treated on equal footing. First, a quantum-mechanical model for HC generation is developed. Its connection to existing semiclassical models and time-dependent density functional theory (TDDFT) is discussed. Second, the relaxation and lifetimes of HCs are investigated in the presence of electron–electron and electron–phonon interactions. A GW-like approximation is introduced to account for the electron–electron scattering. The numerical simulations on the Jellium nanoparticles with a size up to 1.6 nm demonstrate the electron–electron scattering and electron–phonon scattering dominate different time scale in the relaxation dynamics. We also generalize the model to study the extraction of HCs to attached molecules. The quantum yield of extracting HCs for other applications is found to be size-dependent. In general, the smaller size of NP improves the quantum yield, which is in agreement with recent experimental measurements. Even though we demonstrate this newly developed theoretical formalism with Jellium model, the theory applies to any other atomistic models.

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

Overview of the physics basis for the ARC fusion power plant

Commonwealth Fusion Systems plans to build ARC as the first fusion power plant at a site in Chesterfield County, Virginia, USA by the early 2030s. We present an overview of analysis comprising the physics basis of the ARC V3A design, a high-magnetic-field tokamak with 𝐵 0 =11.4 T, 𝐼 𝑝 =12.0 MA, 𝑅 0 =4.62 m, 𝑎 =1.18 m. ARC V3A is designed to produce 𝑃 𝑓⁡𝑢⁢𝑠 ≈1.13 GW DT fusion power and deliver ⩾400 MW net electric power to the grid. This overview includes quantitative analysis of fundamental issues for design of and operational plasma scenarios for a tokamak power plant, and lays out the design targets and strategic choices for ARC, including empirical fusion performance projections, assessment of H-mode access, ion cyclotron resonance heating simulations, alpha particle physics and time-dependent full-pulse simulations. This is complemented by topical papers on fusion performance and transport, disruption physics, boundary physics and magnetohydrodynamic stability. Critically, these studies identify key model uncertainties and physics risks to be retired through SPARC operation. Due to the modular nature of ARC, early results from SPARC can be incorporated into the design of the first ARC as well as subsequent replacements of the ARC vacuum vessel.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

All-electron ab initio Bethe-Salpeter equation approach to neutral excitations in molecules with numeric atom-centered orbitals

The Bethe-Salpeter equation (BSE) based on GW quasiparticle levels is a successful approach for calculating the optical gaps and spectra of solids and also for predicting the neutral excitations of small molecules. We here present an all-electron implementation of the GW+BSE formalism for molecules, using numeric atom-centered orbital (NAO) basis sets. We present benchmarks for low-lying excitation energies for a set of small organic molecules, denoted in the literature as “Thiel’s set.” Literature reference data based on Gaussian-type orbitals are reproduced to about one millielectron-volt precision for the molecular benchmark set, when using the same GW quasiparticle energies and basis sets as the input to the BSE calculations. For valence correlation consistent NAO basis sets, as well as for standard NAO basis sets for ground state density-functional theory with extended augmentation functions, we demonstrate excellent convergence of the predicted low-lying excitations to the complete basis set limit. A simple and affordable augmented NAO basis set denoted “tier2+aug2” is recommended as a particularly efficient formulation for production calculations. We finally demonstrate that the same convergence properties also apply to linear-response time-dependent density functional theory within the NAO formalism.

Liu, Chi↗
DOE OSTI2025

𝐴𝑏 initio density-matrix approach to exciton coherence: Phonon scattering, Coulomb interactions, and radiative recombination

Relaxation processes following light excitation in semiconductors are key in materials-based quantum technology applications. These processes are broadly studied in atomically thin transition-metal dichalcogenides, quasi-two-dimensional excitonic semiconductors in which atomistic design allows for tunable excited-state properties, such as relaxation lifetimes and photoinduced coherence. In this work, we present a density-matrix-based approach to compute exciton relaxation within a many-body ab initio perspective. We expand our previously developed Lindblad density-matrix formalism to capture multichannel electron-hole pair relaxation processes, including phonon and Coulomb scattering as well as radiative recombination, and we study their effect on the time-resolved excited-state propagation. Using monolayer MoSe 2 as a prototypical example, we examine many-body effects on the time-dependent dynamics of photoactive excitations, exploring how the electron-hole pair interactions are reflected in variations of the excitation energy, spectral signature, and state coherence. In conclusion, our method supplies a detailed understanding of exciton relaxation mechanisms in realistic materials, offering a previously unexplored pathway to study excited-state dynamics in semiconductors from first principles.

Band structure methods↗
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↗