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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Theoretical prediction of magnetic exchange coupling constants from broken-symmetry coupled cluster calculations

Exchange coupling constants ( J ) are fundamental to the understanding of spin spectra of magnetic systems. In this study, we investigate the broken-symmetry (BS) approaches of Noodleman and Yamaguchi in conjunction with coupled cluster (CC) methods to obtain exchange couplings. J values calculated from CC in this fashion converge smoothly toward the full configuration interaction result with increasing level of CC excitation. We compare this BS-CC scheme to the complementary equation-of-motion CC approach on a selection of bridged molecular cases and give results from a few other methodologies for context.

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

Resource-Efficient Chemistry on Quantum Computers with the Variational Quantum Eigensolver and The Double Unitary Coupled-Cluster approach

Applications of quantum simulation algorithms to obtain electronic energies of molecules on noisy intermediate-scale quantum (NISQ) devices require careful consideration of resources describing the complex electron correlation effects. In modeling second-quantized problems, the biggest challenge confronted is that the number of qubits scales linearly with the size of molecular basis. This poses a significant limitation on the size of the basis sets and the number of correlated electrons included in quantum simulations of chemical processes. To address this issue and to enable more realistic simulations on NISQ computers, we employ the double unitary coupled-cluster (DUCC) method to effectively downfold correlation effects into the reduced-size orbital space, commonly referred to as the active space. Using downfolding techniques, we demonstrate that properly constructed effective Hamiltonians can capture the effect of the whole orbital space in small-size active spaces. Combining the downfolding pre-processing technique with the Variational Quantum Eigensolver, we solve for the ground-state energy of H2 and Li2 in the cc-pVTZ basis using the DUCC-reduced active spaces. We compare these results to full configuration-interaction and high-level coupled-cluster reference calculations.

quantum computing, variational quantum solver, cou↗
DOE OSTI2022

Molecular Polaritonics: Chemical Dynamics Under Strong Light–Matter Coupling

Chemical manifestations of strong light–matter coupling have recently been a subject of intense experimental and theoretical studies. Here we review the present status of this field. Section 1 is an introduction to molecular polaritonics and to collective response aspects of light–matter interactions. Section 2 provides an overview of the key experimental observations of these effects, while Section 3 describes our current theoretical understanding of the effect of strong light–matter coupling on chemical dynamics. A brief outline of applications to energy conversion processes is given in Section 4. Pending technical issues in the construction of theoretical approaches are briefly described in Section 5. Finally, the summary in Section 6 outlines the paths ahead in this exciting endeavor.

Chemistry↗
DOE OSTI2024

Numerical coupling of aerosol emissions, dry removal, and turbulent mixing in the E3SM Atmosphere Model version 1 (EAMv1) – Part 1: Dust budget analyses and the impacts of a revised coupling scheme

Abstract. An earlier study evaluating dust life cycle in the Energy Exascale Earth System Model (E3SM) Atmosphere Model version 1 (EAMv1) has revealed that the simulated global mean dust lifetime is substantially shorter when higher vertical resolution is used, primarily due to significant strengthening of dust dry removal in source regions. This paper demonstrates that the sequential splitting of aerosol emissions, dry removal, and turbulent mixing in the model's time integration loop, especially the calculation of dry removal after surface emissions and before turbulent mixing, is the primary reason for the vertical resolution sensitivity reported in that earlier study. Based on this reasoning, we propose a revised numerical process coupling scheme that requires the least amount of code changes, in which the surface emissions are applied before turbulent mixing instead of before dry removal. The revised scheme allows newly emitted particles to be transported aloft by turbulence before being removed from the atmosphere, and hence better resembles the dust life cycle in the real world. Sensitivity experiments show that the revised process coupling substantially weakens dry removal and strengthens vertical mixing in dust source regions. It also strengthens the large-scale transport from source to non-source regions, strengthens dry removal outside the source regions, and strengthens wet removal and activation globally. In transient simulations of the years 2000–2009 conducted using 1∘ horizontal grid spacing, 72 vertical layers, and unchanged tuning parameters of emission strength, the revised process coupling leads to a 40 % increase in the global total dust burden and an increase of dust lifetime from 1.8 to 2.5 d in terms of 10-year averages. Weakened dry removal and increased mixing ratios are also seen for other aerosol species that have substantial surface emissions, although the changes in mixing ratio are considerably smaller for the submicron species than for dust and sea salt. Numerical experiments confirm that the revised coupling scheme significantly reduces the strong and non-physical sensitivities of model results to vertical resolution in the original EAMv1. This provides a motivation for adopting the revised scheme in EAM as well as for further improvements on the simple revision presented in this paper.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2023

Fast Coupled Loads Analysis Method: Norton-Thevenin Receptance Coupling

A new method called Norton-Thevenin Receptance Coupling (NTRC) has been developed to perform coupled loads analysis (CLA). NTRC provides a tool that payload developers can use to obtain launch loads at a fraction of the cost of a CLA any time it is required in the payload design cycle. NTRC combines the frequency domain component coupling method of Receptance Coupling with the Norton and Thevenin theory used in force limiting to derive an alternate method for performing CLA.

Coupled Loads Analysis↗
DOE OSTI2019

Effects of electron-phonon coupling and electronic thermal conductivity in high energy molecular dynamics simulations of irradiation cascades in nickel

The two-temperature model has been applied to investigate the effects of the electronic subsystem on 150 keV Ni ion cascades in nickel using molecular dynamics simulation. We explore the effects of the magnitude of the electron-phonon coupling and the electronic thermal conductivity on defect production and cluster formation. It has been found that stronger electron-phonon coupling allows larger and more rapid energy feedback to the atomic subsystem, leading to reduction of number of point defects and suppression of the formation of larger defect clusters. It was observed that larger electronic thermal conductivity results in slightly increased number of point defects and larger size vacancy clusters. The latter takes place because of suppression of point defects recombination in faster cooling areas of initial damage.

Zarkadoula, Eva↗
DOE OSTI2020

Electronically Coupled 2D Polymer/MoS 2 Heterostructures

Emergent quantum phenomena in electronically coupled two-dimensional heterostructures are central to next-generation optical, electronic, and quantum information applications. Tailoring electronic band gaps in coupled heterostructures would permit control of such phenomena and is the subject of significant research interest. Two-dimensional polymers (2DPs) offer a compelling route to tailored band structures through the selection of molecular constituents. However, despite the promise of synthetic flexibility and electronic design, fabrication of 2DPs that form electronically coupled 2D heterostructures remains an outstanding challenge. Here, we report the rational design and optimized synthesis of electronically coupled semiconducting 2DP/2D transition metal dichalcogenide van der Waals heterostructures, demonstrate direct exfoliation of the highly crystalline and oriented 2DP films down to a few nanometers, and present the first thickness-dependent study of 2DP/MoS 2 heterostructures. In this work, control over the 2DP layers reveals enhancement of the 2DP photoluminescence by two orders of magnitude in ultrathin sheets and an unexpected thickness-dependent modulation of the ultrafast excited state dynamics in the 2DP/MoS 2 heterostructure. These results provide fundamental insight into the electronic structure of 2DPs and present a route to tune emergent quantum phenomena in 2DP hybrid van der Waals heterostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Theoretical Study of C-H Bond Cleavage via Concerted Proton-Coupled Electron Transfer in Fluorenyl-Benzoates

Developing new strategies to activate and cleave C-H bonds is important for a broad range of applications. Recently a new approach for C-H bond activation using multi-site concerted proton-coupled electron transfer (PCET) involving intermolecular electron transfer to an oxidant coupled to intramolecular proton transfer was reported. For a series of oxidants reacting with 2-(9H-fluoren-9-yl)benzoate, experimental studies revealed an atypical Brønsted a, defined as the slope of the logarithm of the PCET rate constant versus the logarithm of the equilibrium constant or the scaled driving force. Herein this reaction is modeled with a vibronically nonadiabatic PCET theory. Hydrogen tunneling, thermal sampling of the proton donor-acceptor mode, solute and solvent reorganization, and contributions from excited vibronic states are found to play important roles. The calculations qualitatively reproduce the experimental observation of a Brønsted a significantly less than 0.5 and explain this shallow slope in terms of exoergic processes between pairs of electron-proton vibronic states. These fundamental mechanistic insights may guide the design of more effective strategies for C-H bond activation and cleavage.

Sayfutyarova, Elvira R.↗
DOE OSTI2022

Internal conversion and intersystem crossing dynamics based on coupled potential energy surfaces with full geometry-dependent spin–orbit and derivative couplings. Nonadiabatic photodissociation dynamics of NH 3 (A) leading to the NH(X 3 Σ – , a 1 Δ) + H 2 channel

Here we simulate the photodissociation of NH 3 originating from its first excited singlet state S 1 into the NH 2 + H (radical) and NH + H 2 (molecular) channels. The states considered are the ground singlet state S 0 , the first excited singlet state S 1 and the lowest-lying triplet state T 1 , which permit for the first time a uniform treatment of the internal conversion and intersystem crossing. The simulations are based on a diabatic potential energy matrix (DPEM) of S 0 , S 1 coupled by a conical intersection seam, as well as a potential energy surface (PES) for T 1 coupled by spin-orbit coupling (SOC) to the two singlet states. The DPEM and PES are fitted to ab initio electronic structure data (ESD) including energies, energy gradients, and derivative couplings. The DPEM also defines an adiabatic to diabatic state (AtD) transformation, which is used to transform the singular adiabatic SOC into a smooth function of the nuclear coordinates in the diabatic representation, allowing the diabatic SOC to be fit to an analytical functional form. ESD and SOC data obtained from these surfaces can serve as input for either quantum or semi-classical characterization of the nonadiabatic dynamics. Using the SHARC suite of programs, nonadiabatic simulations based on over 40 000 semi-classical trajectories assess the convergence of our results. The production of NH + H 2 is not direct, but is only achieved through a quasi-statistical dissociation mechanism after internal conversion to the ground electronic state. This leads to a much lower yield comparing with the main NH 2 + H channel. The NH(X 3 Σ_) radical produced through the intersystem crossing from S 0 to T 1 is rare (~0.2%) compared to NH(a 1 Δ) due to the process being spin forbidden.

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

Recent advances in coupled cluster computations of open-shell atomic nuclei

In this contribution, we report on recent progress in coupled-cluster simulations of open-shell atomic nuclei using interactions consistently derived from chiral effective field theory. In particular, we compare different coupled-cluster approaches by computing binding energies and electric dipole polarizabilities in medium-mass calcium isotopes.

Marino, Francesco [Johannes Gutenberg Univ., Mainz↗
DOE OSTI2019

Direct diabatization and analytic representation of coupled potential energy surfaces and couplings for the reactive quenching of the excited 2 Σ + state of OH by molecular hydrogen

In this work, we have employed extended multiconfiguration quasidegenerate perturbation theory, fourfold-way diabatic molecular orbitals, and configurational uniformity to develop a global three-state diabatic representation of the potential energy surfaces and their couplings for the electronically nonadiabatic reaction OH* + H 2 → H 2 O + H, where * denotes electronic excitation to the A 2 Σ + state. To achieve sign consistency of the computed diabatic couplings, we developed a graphics processing unit-accelerated algorithm called the cluster-growing algorithm. Having obtained consistent signs of the diabatic couplings, we fit the diabatic matrix elements (which consist of the diabatic potentials and the diabatic couplings) to analytic representations. Adiabatic potential energy surfaces are generated by diagonalizing the 3 × 3 diabatic potential energy matrix. The comparisons between the fitted and computed diabatic matrix elements and between the originally computed adiabatic potential energy surfaces and those generated from the fits indicate that the current fit is accurate enough for dynamical studies, and it may be used for quantal or semiclassical dynamics calculations.

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

A kinetic model of friction in strongly coupled strongly magnetized plasmas

Plasmas that are strongly magnetized in the sense that the gyrofrequency exceeds the plasma frequency exhibit novel transport properties that are not well understood. As a representative example, we compute the friction force acting on a massive test charge moving through a strongly coupled and strongly magnetized one-component plasma using a generalized Boltzmann kinetic theory. Recent works studying the weakly coupled regime have shown that strong magnetization leads to a transverse component of the friction force that is perpendicular to both the Lorentz force and velocity of the test charge, in addition to the stopping power component aligned antiparallel to the velocity. Recent molecular dynamics simulations have also shown that strong Coulomb coupling in addition to strong magnetization gives rise to a third component of the friction force in the direction of the Lorentz force. Here, we show that the generalized Boltzmann kinetic theory captures these effects and generally agrees well with the molecular dynamics simulations over a broad range of Coulomb coupling and magnetization strength regimes. The theory is also used to show that the “gyro” component of the friction in the direction of the Lorentz force arises due to asymmetries associated with gyromotion during short-range collisions. Computing the average motion of the test charge through the background plasma, the transverse force is found to strongly influence the trajectory by changing the gyroradius and the gyrofriction force is found to slightly change the gyrofrequency of the test charge resulting in a phase shift.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Optimal control of coupled quantum systems based on the first-order Magnus expansion: Application to multiple dipole-dipole-coupled molecular rotors

This paper presents a method for performing approximate optimal control simulations for quantum systems with multiple coupled degrees of freedom. In this work, the time evolution is simulated using the first-order Magnus expansion in the interaction picture, where the couplings between different degrees of freedom are treated as the perturbation. A numerical implementation procedure is presented that leverages upon pairwise couplings and the separability of the zeroth-order time evolution operator to achieve a reduced computational cost, which is analyzed with respect to the number of degrees of freedom. The formulation is compatible with gradient-free methods to optimize the control field, and a stochastic hill climbing algorithm is adopted for this purpose. As illustrations, optimal control simulations are performed for systems of two and three dipole-dipole-coupled molecular rotors under the influence of a control field. For the two-rotor system, the field is optimized to achieve either orientation or entanglement objectives. For the three-rotor system, the field is optimized either to orient all three rotors in the same direction or to orient one rotor in a particular direction while the other two rotors point in the opposite direction.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Local imaging of diamagnetism in proximity-coupled niobium nanoisland arrays on gold thin films.

In this work, we study the effect of engineered disorder on the local magnetic response of proximity-coupled superconducting island arrays by comparing scanning superconducting quantum interference device (SQUID) susceptibility measurements to a model in which we treat the system as a network of one-dimensional (1D) superconductor-normal-metal-superconductor Josephson junctions, each with a Josephson coupling energy E-J determined by the junction length or distance between islands. We find that the disordered arrays exhibit a spatially inhomogeneous diamagnetic response which, for low local applied magnetic fields, is well described by this junction network model, and we discuss these results as they relate to inhomogeneous 2D superconductors. Our model of the static magnetic response of the arrays does not fully capture the onset of nonlinearity and dissipation with increasing applied field, as these effects are associated with vortex motion due to the dynamic nature of the scanning SQUID susceptometry measurement. This work demonstrates a model 2D superconducting system with engineered disorder, and it highlights the impact of dissipation on the local magnetic properties of 2D superconductors and Josephson junction arrays.

Bishop-Van Horn, Logan↗