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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 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Polar liquids at charged interfaces: A dipolar shell theory

The structure of polar liquids and electrolytic solutions, such as water and aqueous electrolytes, at interfaces underlies numerous phenomena in physics, chemistry, biology, and engineering. In this work, we develop a continuum theory that captures the essential features of dielectric screening by polar liquids at charged interfaces, including decaying spatial oscillations in charge and mass, starting from the molecular properties of the solvent. The theory predicts an anisotropic dielectric tensor of interfacial polar liquids previously studied in molecular dynamics simulations. We explore the effect of the interfacial polar liquid properties on the capacitance of the electrode/electrolyte interface and on hydration forces between two plane-parallel polarized surfaces. In the linear response approximation, we obtain simple formulas for the characteristic decay lengths of molecular and ionic profiles at the interface.

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

Probing atomic physics at ultrahigh pressure using laser-driven implosions

Abstract Spectroscopic measurements of dense plasmas at billions of atmospheres provide tests to our fundamental understanding of how matter behaves at extreme conditions. Developing reliable atomic physics models at these conditions, benchmarked by experimental data, is crucial to an improved understanding of radiation transport in both stars and inertial fusion targets. However, detailed spectroscopic measurements at these conditions are rare, and traditional collisional-radiative equilibrium models, based on isolated-atom calculations and ad hoc continuum lowering models, have proved questionable at and beyond solid density. Here we report time-integrated and time-resolved x-ray spectroscopy measurements at several billion atmospheres using laser-driven implosions of Cu-doped targets. We use the imploding shell and its hot core at stagnation to probe the spectral changes of Cu-doped witness layer. These measurements indicate the necessity and viability of modeling dense plasmas with self-consistent methods like density-functional theory, which impact the accuracy of radiation transport simulations used to describe stellar evolution and the design of inertial fusion targets.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Testing $f(R)$ gravity with scale dependent cosmic void velocity profiles

Here, we study the impact of cosmological scale modifications to general relativity on the dynamics of halos within voids by comparing N-body simulations incorporating Hu-Sawicki f(R) gravity, with |f R0 | = 10 -6 and 10 -5 , to those of Λ CDM. By examining the radial velocity statistics within voids classified based on their size and density-profile, as “rising” (R-type) or “shell” (S-type), we find that halo motions in small R-type voids, with effective radius <15 Mpc/h, reveal distinctive differences between f(R) and Λ CDM cosmologies. To understand this observed effect, we study the linear and nonlinear fifth forces, and develop an iterative algorithm to accurately solve the nonlinear fifth force equation. We use this to characterize the Chameleon screening mechanism in voids and contrast the behavior with that observed in gravitationally collapsed objects. The force analysis underscores how smaller R-type voids exhibit the highest ratios of fifth force to Newtonian force, which source distinguishable differences in the velocity profiles and thereby provide rich environments in which to constrain gravity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Energetics and kinetics of various cyano radical hydrogen abstractions

The cyano radical (CN) is an abundant, open-shell molecule found in a variety of environments, including the atmosphere, the interstellar medium and combustion processes. In these environments, it often reacts with small, closed-shell molecules via hydrogen abstraction. Both carbon and nitrogen atoms of the cyano radical are reactive sites, however the carbon is more reactive with reaction barrier heights generally between 2–15 kcal mol -1 lower than those of the analogous nitrogen. The CN + HX → HCN/HNC + X, with X = H, CH 3 , NH 2 , OH, F, SiH 3 , PH 2 , SH, Cl, C 2 H, CN reactions have been studied at a high-level of theory, including CCSD(T)-F12a. Finally, kinetics were obtained over the 100–1000 K temperature range, showing excellent agreement with those rate constants that have been determined experimentally.

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

Density Functional Tight Binding Insights into Plasmonic Silver–Platinum Nanoparticles and Alloys for Enhanced Photocatalysis

Developing accurate and efficient Slater-Koster (SK) tight-binding parameter sets is essential for quantum plasmonic studies of alloyed metal nanoparticles, as conventional time dependent density functional theory (TD-DFT) calculations are computationally prohibitive for larger clusters. In this work, we develop and validate density functional tight binding (DFTB) parameter sets for both ground state (GS-SK) and excited state (ES-SK) calculations to study the structural, electronic, and optical properties of silver (Ag), platinum (Pt), and Ag–Pt nanoalloys. Our investigation of the ground state properties demonstrates that the GS-SK parameters enable DFTB to closely reproduce the electronic structures of platinum clusters with diverse sizes and geometries – showing qualitative agreement with DFT for density of states (DOS) profiles and energy levels. The ES-SK parameters accurately describe excited-state properties compared to TD-DFT reference calculations, including the broad, featureless absorption profiles of Pt that are dominated by interband transitions. Using the ES-SK parameters within a real-time TD-DFTB framework, we compute size-dependent optical absorption spectra of Ag, Pt and Ag-Pt nanocubes containing up to 1099 atoms (size ∼4.18 nm). A detailed study of Ag–Pt and Pt-Ag core–shell nanoparticles shows quenching of the Ag plasmon resonance even at monolayer coverage for Ag-Pt, but not for Pt-Ag. We also show how to define submonolayer Ag-core Pt-shell cubic structures that have similar optical properties to those generated experimentally for much larger particles, which offers potential for describing plasmon-enhanced photocatalysis. Collectively, the GS-SK and ES-SK parameter sets provide an accurate, computationally efficient approach for modeling the complex optical and electronic behavior of noble–transition metal nanostructures and their alloys.

SPR↗
DOE OSTI2025

Modular-Invariant Random Matrix Theory and AdS 3 Wormholes

We develop a nonperturbative definition of RMT 2 : a generalization of random matrix theory that is compatible with the symmetries of two-dimensional conformal field theory. Given any random matrix ensemble, its 𝑛-point spectral correlations admit a prescribed modular-invariant lift to RMT 2 , which moreover reduce to the original random matrix correlators in a near-extremal limit. Central to the prescription is a presentation of random matrix theory in Mellin space, which lifts to two dimensions via the SL⁡(2,ℤ) spectral decomposition employed in previous work. As a demonstration we perform the explicit RMT 2 lift of two-point correlations of the GUE Airy model. We propose that in AdS 3 pure gravity, semiclassical amplitudes for off-shell 𝑛-boundary torus wormholes with topology Σ 0,𝑛 × 𝑆 1 are given by the RMT 2 lift of JT gravity wormhole amplitudes. For the three-boundary case, we identify a gravity calculation which matches the RMT 2 result.

conformal field theory↗
DOE OSTI2023

Schematic model for induced fission in a configuration-interaction approach

We model fission at barrier-top energies in a simplified model space that permits comparison of different components of the residual nucleon-nucleon interaction. The model space is built on particle-hole excitations of reference configurations. These are Slater determinants of uniformly spaced orbitals characterized only by their quantum numbers and orbital energies. The residual interaction in the Hamiltonian includes the diabatic interaction connecting similar orbitals at different deformations, the pairing interaction between like nucleons, and a schematic off-diagonal neutron-proton interaction. We find that the fission reaction probability is sensitive to the off-diagonal neutron-proton interaction much more than to the pairing and the diabatic interactions. In particular, the transmission coefficients become insensitive to the strength of the pairing interaction when the neutron-proton interaction is large. Here, we also find that the branching ratio is insensitive to the final-state scission dynamics, as is assumed in the well-known Bohr-Wheeler theory.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Leading-order gravitational radiation to all spin orders

Starting with on-shell amplitudes compatible with the scattering of Kerr black holes up to Compton-amplitude contact terms, we produce the gravitational waveform and memory effect including spin at their leading post-Minkowskian orders to all orders in the spins of both scattering objects. For the memory effect, we present results at next-to-leading order as well, finding a closed form for all spin orders when the spins are anti-aligned and equal in magnitude. Considering instead generically oriented spins, we produce the next-to-leading-order memory to sixth order in spin. Compton-amplitude contact terms up to sixth order in spin are included throughout our analysis.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Near conformal perturbation theory in SYK type models

We present a systematic procedure to extract the dynamics of the low energy soft mode in SYK type models with a single energy scale J and emergent reparametrization symmetry in the IR. This is given in the framework of the perturbative scheme of arXiv:1608.07567 based on a specific (off-shell) breaking of conformal invariance in the UV, adjusted to yield the exact large-N saddle point. While this breaking term formally vanishes on-shell, it has a non-trivial effect on correlation functions and the effective action. In particular, it leads to the Schwarzian action with a specific coupling to bi-local matter. The method is applied to the evaluation of O(1) corrections to the correlation function of bi-locals. As a byproduct we confirm precise agreement with the explicit, symmetry breaking procedure. We provide a verification in the large q limit (Liouville theory), where the correlators can be calculated exactly at all length scales. In this case, our scheme illuminates how the enhanced O(J) and the subleading O(1) contributions originate from the Schwarzian dynamics of the soft mode and its interaction with h = 2 (bi-local) matter.

1/N expansion↗
DOE OSTI2021

Fermi acceleration in relativistic collisionless plasma shocks correlates with anisotropic energy gains

Collisionless shocks generated by two colliding relativistic electron-positron plasma shells are studied using particle-in-cell simulations. Shocks are mediated by the Weibel instability (WI), and the kinetic energy of the fastest accelerated particles is found to be anisotropically modified by WI-induced electric fields. Specifically, we show that all particles interacting with the shock bifurcate into two groups based on their final relativistic Lorentz factor γ: slow (γ < γ bf ) and fast (γ < γ bf ), where γ bf is the bifurcation Lorentz factor that was found to be approximately twice the initial (upstream) Lorentz factor γ0. We have found that the kinetic energies of the slow particles are equally affected by the longitudinal and transverse components of the shock electric field, whereas the fast particles are primarily accelerated by the transverse field component.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Hybridizing pseudo-Hamiltonians and non-local pseudopotentials in diffusion Monte Carlo

An accurate treatment of effective core potentials (ECPs) requires care in continuum quantum Monte Carlo (QMC) methods. While most QMC studies have settled on the use of familiar non-local (NL) pseudopotentials with additional localization approximations, these approaches have been shown to result in moderate residual errors for some classes of molecular and solid state applications. Here, we revisit an idea proposed early in the history of QMC ECPs that does not require localization approximations, namely, a differential class of potentials referred to as pseudo-Hamiltonians. We propose to hybridize NL potentials and pseudo-Hamiltonians to reduce residual non-locality of existing potentials. We derive an approach to recast pseudopotentials for 3d elements as hybrid pseudo-Hamiltonians with optimally reduced NL energy. We demonstrate the fidelity of the hybrid potentials by studying atomic ionization potentials of Ti and Fe and the binding properties of TiO and FeO molecules with diffusion Monte Carlo (DMC). We show that localization errors have been reduced relative to potentials with the same NL channels for Sc–Zn by considering the DMC energy change with respect to the choice of approximate localization. While localization error decreases proportionate to the reduced NL energy without a Jastrow, with a Jastrow, the degree of reduction decreases at higher filling of the d-shell. Our results suggest that a subset of existing ECPs may be recast in this hybrid form to reduce the DMC localization error. They also point to the prospect of further reducing this error by generating ECPs within this hybrid form from the start.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Solvent Dynamics Are Critical to Understanding Carbon Dioxide Dissolution and Hydration in Water

Simulations of carbon dioxide (CO 2 ) in water may aid in understanding the impact of its accumulation in aquatic environments and help advance technologies for carbon capture and utilization (via, e.g., mineralization). Quantum mechanical (QM) simulations based on static molecular models with polarizable continuum solvation poorly reproduce the energetics of CO 2 hydration to form carbonic acid in water, independent of the level of QM theory employed. Only with density-functional-theory-based molecular dynamics and rare-event sampling, followed by energy corrections based on embedded correlated wavefunction theory (in conjunction with density functional embedding theory), can a close agreement between theory and experiment be achieved. Such multilevel simulations can serve as benchmarks for simpler, less costly models, giving insight into potential errors of the latter. The strong influence of sampling/averaging over dynamical solvent configurations on the energetics stems from the difference in polarity of both the transition state and product (both polar) versus the reactant (nonpolar). When a solute undergoes a change in polarity during reaction, affecting its interaction with the solvent, careful assessment of the energetic contribution of the solvent response to this change is critical. Here, we show that static models (without structural sampling) that incorporate three explicit water molecules can yield far superior results than models with more explicit water molecules because fewer water molecules yield less configurational artifacts. Static models intelligently incorporating both explicit (molecules directly participating in the reaction) and implicit solvation, along with a proper QM theory, e.g., CCSD(T) for closed-shell systems, can close the accuracy gap between static and dynamic models.

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

Reexamining the variational two-particle reduced density matrix for nuclear systems

We report that in most nuclear many-body methods, observables are calculated using many-body wave functions explicitly. The variational two-particle reduced density matrix method is one of the few exceptions to the rule. Ground-state energies of both closed-shell and open-shell nuclear systems can indeed be evaluated by minimizing a constrained linear functional of the two-particle reduced density matrix. However, it has virtually never been used in nuclear theory, because nuclear ground states were found to be well overbound, contrary to those of atoms and molecules. Consequently, we introduced new constraints in the nuclear variational two-particle reduced density matrix method, developed recently for atomic and molecular systems. Our calculations then show that this approach can provide a proper description of nuclear systems where only valence neutrons are included. For the nuclear systems where both neutrons and protons are active, however, the energies obtained with the variational two-particle reduced density matrix method are still overbound. The possible reasons for the noticed discrepancies and solutions to this problem will be discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Perspective on Kramers symmetry breaking and restoration in relativistic electronic structure methods for open-shell systems

Without rigorous symmetry constraints, solutions to approximate electronic structure methods may artificially break symmetry. In the case of the relativistic electronic structure, if time-reversal symmetry is not enforced in calculations of molecules not subject to a magnetic field, it is possible to artificially break Kramers degeneracy in open shell systems. This leads to a description of excited states that may be qualitatively incorrect. Despite this, different electronic structure methods to incorporate correlation and excited states can partially restore Kramers degeneracy from a broken symmetry solution. For single-reference techniques, the inclusion of double and possibly triple excitations in the ground state provides much of the needed correction. Formally, however, this imbalanced treatment of the Kramers-paired spaces is a multi-reference problem, and so methods such as complete-active-space methods perform much better at recovering much of the correct symmetry by state averaging. Using multi-reference configuration interaction, any additional corrections can be obtained as the solution approaches the full configuration interaction limit. A recently proposed “Kramers contamination” value is also used to assess the magnitude of symmetry breaking.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Impact of the MARATHON data on F 2⁢n⁡ /F 2⁢p and off-shell effects in light nuclei

The neutron structure function, F 2⁢n⁡ , has historically been extracted from measurements of the deuteron structure function, which is limited by our understanding of the nuclear effects on the bound proton and neutron. The MARATHON Collaboration recently extracted F 2⁢n⁡ from the comparison of 3 H and 3 He targets, where the nuclear effects are larger but nearly identical, yielding a precise extraction of F 2⁢n⁡ /F 2⁢p . Here, to ensure that this comparison is not biased by the specific model of nuclear effects used by MARATHON, we examine a range of models of the nuclear effects to obtain a more conservative, but more model-independent, extraction of F 2⁢n⁡ /F 2⁢p for comparison with deuteron extractions. Even with this approach, the results are precise enough to compare to deuteron extractions, providing new constraints on the nuclear effects in the deuteron and indicating the need for larger nuclear corrections than those included in most models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

$t\bar{t}b\bar{b}$ at the LHC: on the size of corrections and b -jet definitions

We report on the calculation of the next-to-leading order QCD corrections to the production of a $t\bar t$ pair in association with two heavy-flavour jets. We concentrate on the di-lepton $t\bar t$ decay channel at the LHC with $\sqrt{s}$ = 13 TeV. The computation is based on pp → $e^+ν_eμ^-\bar{ν}_μb\bar{b}b\bar{b}$ matrix elements and includes all resonant and non-resonant diagrams, interferences and off-shell effects of the top quark and the W gauge boson. As it is customary for such studies, results are presented in the form of inclusive and differential fiducial cross sections. We extensively investigate the dependence of our results upon variation of renormalisation and factorisation scales and parton distribution functions in the quest for an accurate estimate of the theoretical uncertainties. We additionally study the impact of the contributions induced by the bottom-quark parton density. Results presented here are particularly relevant for measurements of $t\bar{t}H(H → b\bar{b})$ and the determination of the Higgs coupling to the top quark. In addition, they might be used for precise measurements of the top-quark fiducial cross sections and to investigate top-quark decay modelling at the LHC.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Tracking Optical Phonon Dynamics in InP Nanocrystals via Transient Absorption and Femtosecond Stimulated Raman Spectroscopy

Semiconductor nanocrystals (NCs) offer actualized and prospective utility in optoelectronic technologies, yet key aspects of their thermal and vibrational behaviors remain unresolved. Compared with bulk crystals, heat dissipation involving NCs can differ substantially owing to pervasiveness of interfacial scattering, phonon confinement, and relaxed phonon momentum selection rules, as well as influences of ligands. Here, in addition to transient absorption, we use femtosecond stimulated Raman spectroscopy to track nonequilibrium optical-phonon dynamics in InP NCs capped with myristic acid ligands and compare the same particles coated with a ZnS shell. We identify distinct phonon decay pathways in ligand-capped versus ZnS-shelled NCs. Increasing the excitation density and introducing the ZnS shell measurably modify optical-phonon lifetimes, whereas phonon formation times remain largely unchanged. In addition, we observe phonon mode softening in ligand-capped nanocrystals, consistent with lattice expansion. Together, these results demonstrate that core–shell structures can strongly govern nanocrystal thermal dissipation pathways and should be considered a key design parameter for optoelectronic operation.

dissipation↗
DOE OSTI2023

Effects of head modeling errors on the spatial frequency representation of MEG

Abstract Objectives. We aim to investigate the effects of head model inaccuracies on signal and source reconstruction accuracies for various sensor array distances to the head. This allows for the assessment of the importance of head modeling for next-generation magnetoencephalography (MEG) sensors, optically-pumped magnetometers (OPM). Approach. A 1-shell boundary element method (BEM) spherical head model with 642 vertices of radius 9 cm and conductivity of 0.33 S m −1 was defined. The vertices were then randomly perturbed radially up to 2%, 4%, 6%, 8% and 10% of the radius. For each head perturbation case, the forward signal was calculated for dipolar sources located at 2 cm, 4 cm, 6 cm and 8 cm from the origin (center of the sphere), and for a 324 sensor array located at 10 cm to 15 cm from the origin. Equivalent current dipole (ECD) source localization was performed for each of these forward signals. The signal for each perturbed spherical head case was then analyzed in the spatial frequency domain, and the signal and ECD errors were quantified relative to the unperturbed case. Main results. In the noiseless and high signal-to-noise ratio (SNR) case of approximately ≥6 dB, inaccuracies in our spherical BEM head conductor models lead to increased signal and ECD inaccuracies when sensor arrays are placed closer to the head. This is true especially in the case of deep and superficial sources. In the noisy case however, the higher SNR for closer sensor arrays allows for an improved ECD fit and outweighs the effects of head geometry inaccuracies. Significance. OPMs may be placed directly on the head, as opposed to the more commonly used superconducting quantum interference device sensors which must be placed a few centimeters away from the head. OPMs thus allow for signals of higher spatial resolution to be captured, resulting in potentially more accurate source localizations. Our results suggest that an increased emphasis on accurate head modeling for OPMs may be necessary to fully realize its improved source localization potential.

Yeo, Wan-Jin (ORCID:0000000241417123)↗