Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Adiabatic approximation”

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.

At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Scaling and adiabaticity in a rapidly expanding gluon plasma

In this work we aim to gain qualitative insight on the far-from-equilibrium behavior of the gluon plasma produced in the early stages of a heavy-ion collision. It was recently discovered [1] that the distribution functions of quarks and gluons in QCD effective kinetic theory (EKT) exhibit self-similar “scaling” evolution with time-dependent scaling exponents long before those exponents reach their pre-hydrodynamic fixed-point values. In this work we shed light on the origin of this time-dependent scaling phenomenon in the small-angle approximation to the Boltzmann equation. We first solve the Boltzmann equation numerically and find that time-dependent scaling is a feature of this kinetic theory, and that it captures key qualitative features of the scaling of hard gluons in QCD EKT. We then proceed to study scaling analytically and semi-analytically in this equation. We find that an appropriate momentum rescaling allows the scaling distribution to be identified as the instantaneous ground state of the operator describing the evolution of the distribution function, and the approach to the scaling function is described by the decay of the excited states. That is to say, there is a frame in which the system evolves adiabatically. Furthermore, from the conditions for adiabaticity we can derive evolution equations for the time-dependent scaling exponents. In addition to the known free-streaming and BMSS fixed points, we identify a new “dilute” fixed point when the number density becomes small before hydrodynamization. Corrections to the fixed point exponents in the small-angle approximation agree quantitatively with those found previously in QCD EKT and arise from the evolution of the ratio between hard and soft scales.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Toward more accurate adiabatic connection approach for multireference wavefunctions

A multiconfigurational adiabatic connection (AC) formalism is an attractive approach to compute the dynamic correlation within the complete active space self-consistent field and density matrix renormalization group (DMRG) models. Practical realizations of AC have been based on two approximations: (i) fixing one- and two-electron reduced density matrices (1- and 2-RDMs) at the zero-coupling constant limit and (ii) extended random phase approximation (ERPA). This work investigates the effect of removing the “fixed-RDM” approximation in AC. The analysis is carried out for two electronic Hamiltonian partitionings: the group product function- and the Dyall Hamiltonians. Exact reference AC integrands are generated from the DMRG full configuration interaction solver. Two AC models are investigated, employing either exact 1- and 2-RDMs or their second-order expansions in the coupling constant in the ERPA equations. Calculations for model molecules indicate that lifting the fixed-RDM approximation is a viable way toward improving the accuracy of existing AC approximations.

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

Impact of Disorder and Defects on Bond Energies in Highly Fluorinated Graphene

Fluorinated graphite materials are of interest for an assortment of applications and can be synthesized under a variety of synthetic conditions from many different types of carbon. Due to such variations, structural disorders in the form of defects and polymorphism are often present. Here, we investigate the impact of local structural variations on the C–F bond dissociation energies (BDEs) in carbon-based fluoride materials using density functional theory (DFT) computational methods. Employing fluorographene (FG) cluster models, we determine the impact of different C–F bonding configurations in the core of each platelet on the equilibrium BDEs for each C–F bond. The introduction of structural disorder decreases the first C–F BDE by approximately 1 eV compared to the canonical arrangement of axial C–F bonds ordered as in a network of cyclohexane “chairs”. Variability of calculated BDEs among the different polymorphs decreases upon subsequent F removal. Common structural tendencies of the adiabatic defluorination pathways for each polymorph are identified. In conclusion, our analysis suggests that at F/C ratios near 1.0, disorder in the local structure can play a significant role in the energetics of the initial carbon fluoride defluorination and that the influence of this configurational disorder diminishes with decreasing F/C ratios.

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

Vortex Structure of Head Bubble in Convective Cloud Starting Plume

Abstract A developing cumulus cloud (Cu) was modeled, and dynamic, thermodynamic, and microphysical properties of an ascending head bubble reproducing the upper part of a developing Cu were investigated. The data for analysis are taken from 10-m-resolution LES of trade wind Cu under BOMEX conditions. The detection of a rising bubble is carried out using wavelet filtering of the velocity fields and microphysical fields, while a low-frequency signal of the filtering is associated with the convective-scale structure of cloud. We substantiate and discuss the representation of the bubble as a vortex ring, and estimate the parameters of this vortex ring. The simplest Hill’s vortex was chosen as a model of a vortex ring inside cloud. Analytical approximations of the radial profiles of the vertical velocity and of conservative quantities (such as total water mixing ratio and liquid water potential temperature inside and outside the bubble) are obtained. The spatial structure of these quantities is investigated using analytical expressions. Analytical models for spatial distributions of liquid water content (LWC) and adiabatic fraction (AF) are also designed and analyzed. The results demonstrate the existence of a cloud core with high values of LWC and AF up to the height of 1800 m. The horizontally averaged value of the adiabatic fraction, calculated analytically using the Hill’s vortex concept, is evaluated as 0.39, which is the typical AF value in the upper parts of such Cu. The vertical profiles of different important quantities characterizing cloud structure are presented. The analysis performed in this study allows us to conclude that a rising vortex ring plays the dominating role in formation of the thermodynamic and microphysical structure of developing Cu. Significance Statement 1) Dynamic and thermodynamic fields of a developing cumulus cloud simulated by high-resolution LES with spectral bin microphysics are separated into convective and turbulent components by means of the wavelet technique. 2) The analysis of convective component of the cloud revealed the existence of a vortex ring at the developing stage of the cloud and evaluate its parameters. 3) The analysis performed in this study allows us to conclude that a rising vortex ring plays the important role in formation of the thermodynamic and microphysical structure of developing Cu. 4) The study provides a novel insight into the cloud–environment interaction. 5) The approximating equations describing the vortex ring can be usefully applied for developing new schemes of convective parameterization.

Meteorology & Atmospheric Sciences↗
DOE OSTI2022

Conformer-Specific Dissociation Dynamics in Dimethyl Methylphosphonate Radical Cation

The dynamics of the dimethyl methylphosphonate (DMMP) radical cation after production by strong field adiabatic ionization have been investigated. Pump-probe experiments using strong field 1300 nm pulses to adiabatically ionize DMMP and a 800 nm non-ionizing probe induce coherent oscillations of the parent ion yield with a period of about 45 fs. The yields of two fragments, PO 2 C 2 H 7 + and PO 2 CH 4 + , oscillate approximately out of phase with the parent ion, but with a slight phase shift relative to each other. We use electronic structure theory and nonadiabatic surface hopping dynamics to understand the underlying dynamics. The results show that while the cation oscillates on the ground state along the P=O bond stretch coordinate, the probe excites population to higher electronic states that can lead to fragments PO 2 C 2 H 7 + and PO 2 CH 4 + . The computational results combined with the experimental observations indicate that the two conformers of DMMP that are populated under experimental conditions exhibit different dynamics after being excited to the higher electronic states of the cation leading to different dissociation products. These results highlight the potential usefulness of these pump-probe measurements as a tool to study conformer-specific dynamics in molecules of biological interest.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Symmetric Kondo Lattice States in Doped Strained Twisted Bilayer Graphene

We use the topological heavy fermion (THF) model and its Kondo lattice (KL) formulation to study the possibility of a symmetric Kondo (SK) state in twisted bilayer graphene. Via a large-N approximation, we find a SK state in the KL model at fillings v = 0,±1,±2 where a KL model can be constructed. In the SK state, all symmetries are preserved and the local moments are Kondo screened by the conduction electrons. At the mean-field level of the THF model at v = 0,±1,±2,±3 we also find a similar symmetric state that is adiabatically connected to the symmetric Kondo state. We study the stability of the symmetric state by comparing its energy with the ordered (symmetry-breaking) states found in [H. Hu et al., Phys. Rev. Lett. 131, 026502 (2023)., Z.-D. Song and B. A. Bernevig, Phys. Rev. Lett. 129, 047601 (2022).] and find the ordered states to have lower energy at v = 0,±1,±2. However, moving away from integer fillings by doping the light bands, our mean-field calculations find the energy difference between the ordered state and the symmetric state to be reduced, which suggests the loss of ordering and a tendency toward Kondo screening. In order to include many-body effects beyond the mean-field approximation, we also performed dynamical mean-field theory calculations on the THF model in the nonordered phase. The spin susceptibility follows a Curie behavior at v = 0,±1,±2 down to ~2 K where the onset of screening of the local moment becomes visible. This hints to very low Kondo temperatures at these fillings, in agreement with the outcome of our mean-field calculations. At noninteger filling v = ±0.5,±0.8,±1.2 dynamical mean-field theory shows deviations from a 1/T susceptibility at much higher temperatures, suggesting a more effective screening of local moments with doping. Lastly, we study the effect of a C 3⁢z -rotational-symmetry-breaking strain via mean-field approaches and find that a symmetric phase (that only breaks C 3⁢z symmetry) can be stabilized at sufficiently large strain at v = 0,±1,±2. Our results suggest that a symmetric Kondo phase is strongly suppressed at integer fillings, but could be stabilized either at noninteger fillings or by applying strain.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Nonadiabatic transitions during a passage near a critical point

The passage through a critical point of a many-body quantum system leads to abundant nonadiabatic excitations. Here, we explore a regime, in which the critical point is not crossed although the system is passing slowly very close to it. Here, we show that the leading exponent for the excitation probability can then be obtained by standard arguments of the Dykhne formula, but the exponential prefactor is no longer simple and behaves as a power law on the characteristic transition rate. We derive this prefactor for the nonlinear Landau–Zener model by adjusting Dykhne’s approach. Then, we introduce an exactly solvable model of the transition near a critical point in the Stark ladder. We derive the number of excitations for it without approximations and find qualitatively similar results for the excitation scaling.

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

Toward efficient elastocaloric systems: Predicting material thermal properties with high fidelity

A critical need to accurately model thermal behaviors of materials that exhibit strong elastocaloric effects, including predicting the effects themselves at varying stresses and temperatures, has been addressed using a simple and versatile physics-based approach. The key factor leading to the high precision is approximating the underlying elastic phase transition as a smooth modification of lattice entropy between coexisting phases. Once the phase transformation entropy is modeled to match experimentally measured strain as a function of temperature and applied stress, estimating the heat capacity, entropy, and isothermal entropy and adiabatic temperature changes in temperature-stress coordinates becomes straightforward. This approach provides insight into how thermal properties of elastocaloric materials vary through the transition based on strain measurements that are simple to perform and interpret. In addition to aiding in the rapid evaluation of new and existing elastocaloric materials, this advance is expected to prove invaluable for accurate heat transfer modeling aimed at designing efficient regenerative elastocaloric cooling devices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Diabatic quantum annealing for the frustrated ring model

Abstract Quantum annealing (QA) is a continuous-time heuristic quantum algorithm for solving or approximately solving classical optimization problems. The algorithm uses a schedule to interpolate between a driver Hamiltonian with an easy-to-prepare ground state and a problem Hamiltonian whose ground state encodes solutions to an optimization problem. The standard implementation relies on the evolution being adiabatic: keeping the system in the instantaneous ground state with high probability and requiring a time scale inversely related to the minimum energy gap between the instantaneous ground and excited states. However, adiabatic evolution can lead to evolution times that scale exponentially with the system size, even for computationally simple problems. Here, we study whether non-adiabatic evolutions with optimized annealing schedules can bypass this exponential slowdown for one such class of problems called the frustrated ring model. For sufficiently optimized annealing schedules and system sizes of up to 39 qubits, we provide numerical evidence that we can avoid the exponential slowdown. Our work highlights the potential of highly-controllable QA to circumvent bottlenecks associated with the standard implementation of QA.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Lattice holography on a quantum computer

We explore the potential application of quantum computers to the examination of lattice holography, which extends to the strongly coupled bulk theory regime. With adiabatic evolution, we compute the ground state of a spin system on a ( 2 + 1 )-dimensional hyperbolic lattice, and measure the spin-spin correlation function on the boundary. Notably, we observe that with achievable resources for coming quantum devices, the correlation function demonstrates an approximate scale-invariant behavior, aligning with the pivotal theoretical predictions of the anti–de Sitter/conformal field theory correspondence. Published by the American Physical Society 2024

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Observation of subcritical shocks in a collisional laboratory plasma: scale dependence near the resistive length

We present a study of subcritical shocks in a highly collisional laboratory plasma with a dynamically significant magnetic field. Shocks were produced by placing cylindrical obstacles into the supermagnetosonic ( $M_{{\rm MS}} \sim 1.9$ ) outflow from an inverse wire array z-pinch at the MAGPIE pulsed power facility ( $n_{e} \sim 8.5 \times 10^{17}\,{\rm cm}^{-3}$ , $v \sim 45\,{\rm km}\,{\rm s}^{-1}$ ). We demonstrate the existence of subcritical shocks in this regime and find that secondary stagnation shocks form in the downstream which we infer from interferometry and optical Thomson scattering measurements are hydrodynamic in nature. The subcritical shock width is found to be approximately equal to the resistive diffusion length and we demonstrate the absence of a jump in hydrodynamic parameters. Temperature measurements by collective optical Thomson scattering showed little temperature change across the subcritical shock ( ${<}10\,\%$ of the ion kinetic energy) which is consistent with a balance between adiabatic and Ohmic heating and radiative cooling. We demonstrate the absence of subcritical shocks when the obstacle diameter is less than the resistive diffusion length due to decoupling of the magnetic field from the plasma. These findings are supported by magnetohydrodynamic simulations using the Gorgon and AstroBEAR codes and discrepancies between the simulations and experiment are discussed.

Physics↗
DOE OSTI2023

Multimode theory of electron hole transverse instability

We present Vlasov–Poisson three-dimensional linear stability analysis of an initially planar electron hole structure, solving for the distribution function by integration along unperturbed orbits. The non-sinusoidal potential perturbation shape (parallel to $B$ ) is expanded in eigenfunctions of the adiabatic Poisson operator, generalizing the prior assumption of a rigid shift of the equilibrium. We show that the shiftmode is then modified by a second discrete mode plus an integral over a continuum of wave-like modes. A rigorous treatment shows that the continuum can be approximated effectively by a single mode that satisfies the external wave dispersion relation, thus making the perturbation a weighted sum of three modes. We find numerically the solution for the complex instability frequency, and the corresponding three mode amplitudes determining the perturbation eigenmode. This multimode analysis refines the accuracy of the prior single-mode results, giving slightly higher growth rates at most parameters, as expected from the extra mode shape freedom. Oscillating modes near stability boundaries have larger mode distortions which help explain particle-in-cell simulations that observe instability up to ${\sim }20$ % beyond the prior shiftmode thresholds, and narrowing of the perturbation. At high magnetic field, the multimode analysis predicts a reduction of the already small growth rate.

Physics↗
DOE OSTI2025

Evaluating the gradients of localized diabatic state energies and couplings at minimum cost

We calculate the gradients of Boys diabatic state energies and couplings when the electronic vector space is generated by configuration interaction singles. Our approach follows the Lagrangian approach of Paz and Glover (rather than direct differentiation of the adiabatic-to-diabatic approaches that have been published previously). The result is that we achieve a dramatic increase in savings over previous approaches, and the present approach should be immediately useful to scientists focused on electronic relaxation, especially chemists studying electron transfer who wish to go beyond the Condon approximation. Here, a future extension to time-dependent density functional theory in the Tamm–Dancoff approximation is clear.

Chemical physics↗
DOE OSTI2022

Methods to Calculate Electronic Excited-State Dynamics for Molecules on Large Metal Clusters with Many States: Ensuring Fast Overlap Calculations and a Robust Choice of Phase

Here, we present an efficient set of methods for propagating excited-state dynamics involving a large number of configuration interaction singles (CIS) or Tamm-Dancoff approximation (TDA) single-reference excited states. Specifically, (i) following Head-Gordon et al., we implement an exact evaluation of the overlap of singly-excited CIS/TDA electronic states at different nuclear geometries using a biorthogonal basis and (ii) we employ a unified protocol for choosing the correct phase for each adiabat at each geometry. For many-electron systems, the combination of these techniques significantly reduces the computational cost of integrating the electronic Schrodinger equation and imposes minimal overhead on top of the underlying electronic structure calculation. As a demonstration, we calculate the electronic excited-state dynamics for a hydrogen molecule scattering off a silver metal cluster, focusing on high-lying excited states, where many electrons can be excited collectively and crossings are plentiful. Interestingly, we find that the high-lying, plasmon-like collective excitation spectrum changes with nuclear dynamics, highlighting the need to simulate non-adiabatic nuclear dynamics and plasmonic excitations simultaneously. In the future, the combination of methods presented here should help theorists build a mechanistic understanding of plasmon-assisted charge transfer and excitation energy relaxation processes near a nanoparticle or metal surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Effects of collisional ion orbit loss on neoclassical tokamak radial electric fields

Ion orbit loss is considered important for generating the radially inward electric field Er in a tokamak edge plasma. In particular, this effect is emphasized in diverted tokamaks with a magnetic X point. In neoclassical equilibria, Coulomb collisions can scatter ions onto loss orbits and generate a radially outward current, which in steady state is balanced by the radially inward current from viscosity. To quantitatively measure this loss-orbit current in an edge pedestal, an ion-orbit-flux diagnostic has been implemented in the axisymmetric version of the gyrokinetic particle-in-cell code XGC. As the first application of this diagnostic, a neoclassical DIII-D H-mode plasma is studied using gyrokinetic ions and adiabatic electrons. The validity of the diagnostic is demonstrated by studying the collisional relaxation of Er in the core. After this demonstration, the loss-orbit current is numerically measured in the edge pedestal in quasisteady state. In this plasma, it is found that the radial electric force on ions from Er approximately balances the ion radial pressure gradient in the edge pedestal, with the radial force from the plasma flow term being a minor component. The effect of orbit loss on Er is found to be only mild.

gyrokinetic simulations↗
DOE OSTI2025

Lepton flavor asymmetries: from the early Universe to BBN

Large primordial lepton flavor asymmetries with almost vanishing total baryon-minus-lepton number can evade the usual BBN and CMB constraints if neutrino oscillations lead to perfect flavor equilibration. Solving the momentum averaged quantum kinetic equations (QKEs) describing neutrino oscillations and interactions, we perform the first systematic investigation of this scenario, uncovering a rich flavor structure in stark contradiction to the assumption of simple flavor equilibration. We find (i) a particular direction in flavor space, ∆ne ≃ – 2/3 (– 1)∆n μ for normal (inverted) neutrino mass hierarchy, in which the flavor equilibration is efficient and primordial asymmetries are essentially unconstrained, (ii) a minimal washout factor, ∆$n_{e}^{2}$| BBN ≤ 0.03 (0.016) ∑ α ∆$n_{α}^{2}$| ini yielding a conservative estimate for the allowed primordial asymmetries in a generic flavor direction, and (iii) particularly strong or weak washout if one of the initial flavor asymmetries vanishes due to non-adiabatic muon- or electron-driven MSW transitions. These results open up the possibility of a first-order QCD phase transition facilitated by large lepton asymmetries as well as baryogenesis from large and compensated ∆n e = ∆n μ asymmetries. Our systematic approach of deriving momentum averaged QKEs includes collision terms beyond the damping approximation, energy transfer between the neutrino and electron-photon plasma, and provides a fast and reliable way to investigate the impact of primordial lepton asymmetries at the time of BBN. We publicly release the Mathematica code COFLASY-M on https://github.com/mariofnavarro/COFLASY which solves the QKEs numerically.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Effects of collisional ion orbit loss on neoclassical tokamak radial electric fields

We report that ion orbit loss is considered important for generating the radially inward electric field E r in a tokamak edge plasma. In particular, this effect is emphasized in diverted tokamaks with a magnetic X point. In neoclassical equilibria, Coulomb collisions can scatter ions onto loss orbits and generate a radially outward current, which in steady state is balanced by the radially inward current from viscosity. To quantitatively measure this loss-orbit current in an edge pedestal, an ion-orbit-flux diagnostic has been implemented in the axisymmetric version of the gyrokinetic particle-in-cell code XGC. As the first application of this diagnostic, a neoclassical DIII-D H-mode plasma is studied using gyrokinetic ions and adiabatic electrons. The validity of the diagnostic is demonstrated by studying the collisional relaxation of E r in the core. After this demonstration, the loss-orbit current is numerically measured in the edge pedestal in quasisteady state. In this plasma, it is found that the radial electric force on ions from E r approximately balances the ion radial pressure gradient in the edge pedestal, with the radial force from the plasma flow term being a minor component. The effect of orbit loss on E r is found to be only mild.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

ELECTRONIC STRUCTURE METHODS AND PROTOCOLS WITH APPLICATION TO DYNAMICS, KINETICS AND THERMOCHEMISTRY

Hydrocarbon combustion involves the reaction dynamics of a tremendous number of species beginning with many-component fuel mixtures and proceeding via a complex system of intermediates to form primary and secondary products. Combustion conditions corresponding to new advanced engines and/or alternative fuels rely increasingly on autoignition and low-temperature-combustion chemistry. In these regimes various transient radical species such as HO2, ROO·, ·QOOH, HCO, NO2, HOCO, and Criegee intermediates play important roles in determining the detailed as well as more general dynamics. A clear understanding and accurate representation of these processes is needed for effective modeling. Given the difficulties associated with making reliable experimental measurements of these systems, computation can play an important role in developing these energy technologies. Accurate calculations have their own challenges since even within the simplest dynamical approximations such as transition state theory, the rates depend exponentially on critical barrier heights and these may be sensitive to the level of quantum chemistry. Moreover, it is well-known that in many cases it is necessary to go beyond statistical theories and consider the dynamics. Quantum tunneling, resonances, radiative transitions, and non-adiabatic effects governed by spin-orbit or derivative coupling can be determining factors in those dynamics. Building upon progress made during a period of prior support through the DOE Early Career Program, this project combines developments in the areas of potential energy surface (PES) fitting and multistate multireference quantum chemistry to allow spectroscopically and dynamically/kinetically accurate investigations of key molecular systems (such as those mentioned above), many of which are radicals with strong multireference character and have the possibility of multiple electronic states contributing to the observed dynamics. An ongoing area of investigation is to develop general strategies for robustly convergent electronic structure theory for global multichannel reactive surfaces including diabatization of energy and other relevant surfaces such as dipole transition. Combining advances in ab initio methods with automated interpolative PES fitting allows the construction of high-quality PESs (incorporating thousands of high-level data) to be done rapidly through parallel processing on high-performance computing (HPC) clusters. In addition, new methods and approaches to electronic structure theory will be developed and tested through applications. This project will explore limitations in traditional multireference calculations (e.g., MRCI) such as those imposed by internal contraction, lack of high-order correlation treatment and poor scaling. Methods such as DMRG-based extended active-space CASSCF and various Quantum Monte Carlo (QMC) methods will be applied (including VMC/DMC and FCIQMC). Insight into the relative significance of different orbital spaces and the robustness of application of these approaches on leadership class computing architectures will be gained. Synergy with other components of this research program such as automated PES fitting and multireference quantum chemistry will be used to address challenges encountered by the standard approaches to computational thermochemistry (those being single-reference quantum chemistry and perturbative treatments of the anharmonic vibrational energy, which break down for some cases of electronic structure or floppy strongly coupled vibrational modes).

74 ATOMIC AND MOLECULAR PHYSICS↗