Search NASA⌕ Search

SEARCH · Search NASA

Results for “Dynamical correlation”

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 883 records · Page 49
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Quantitative Evaluation of Optical Free Carrier Generation in Semiconducting Single-Walled Carbon Nanotubes

Gauging free carrier generation (FCG) in optically excited, charge-neutral single-walled carbon nanotubes (SWNTs) has important implications for SWNT-based optoelectronics that rely upon conversion of photons to electrical current. Earlier investigations have largely provided only qualitative insights into optically triggered SWNT FCG, due to the heterogeneous nature of commonly interrogated SWNT samples and the lack of direct, unambiguous spectroscopic signatures that could be used to quantify charges. Here, employing ultrafast pump–probe spectroscopy in conjunction with chirality-enriched, length-sorted, ionic-polymer-wrapped SWNTs, we develop a straightforward approach for quantitatively evaluating the extent of optically driven FCG in SWNTs. Owing to the previously identified trion transient absorptive hallmark (Tr + 11 → Tr + nm ) and the rapid nature of trion formation dynamics (<1 ps) relative to established free-carrier decay time scales (>ns), we correlate FCG with trion formation dynamics. Experimental determination of the trion absorptive cross section further enables evaluation of the quantum yields for optically driven FCG [Φ(E nn → h + + e – )] as a function of optical excitation energy and medium dielectric strength. We show that (i) E 33 excitons give rise to dramatically enhanced Φ(E nn → h + + e – ) relative to those derived from E 22 and E 11 excitons and (ii) Φ(E 33 → h + + e – ) monotonically increases from ~5% to 18% as the solvent dielectric constant increases from ~32 to 80. Furthermore, this work highlights the extent to which the nature of the medium and excitation conditions control FCG quantum yields in SWNTs: such studies have the potential to provide new design insights for SWNT-based compositions for optoelectronic applications that include photodetectors and photovoltaics.

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

Alpha-relaxation by scattering and medium-range atomic correlation in simple liquids

The relaxation dynamics of liquid and glass can be studied by inelastic x-ray or neutron scattering through the intermediate scattering function F(Q, t), where Q is the momentum transfer of scattering. Because of the time-consuming nature of these measurements, F(Q, t) is usually measured only at the first peak of the structure function S(Q), and its principal decay time is referred to as the α-relaxation time τ α . τ α is generally considered to describe the relaxation time of the bulk, which is related to viscosity and is controlled by the atomic cage around an atom. Here, through simulations on metallic liquids, we show that the α-relaxation time determined by scattering experiments does not purely reflect viscosity but is influenced by changes in spatial cooperativity. We also demonstrate that atomic caging is not exerted by the nearest neighbors but involves more cooperative atomic dynamics of the atomic medium-range order.

Glass transitions↗
DOE OSTI2019

Spectrum and structure of octet and decuplet baryons and their positive-parity excitations

A continuum approach to the three-valence-quark bound-state problem in quantum field theory, employing parametrizations of the necessary kernel elements, is used to compute the spectrum and Poincare-covariant wave functions for all flavor- SU (3) octet and decuplet baryons and their first positive-parity excitations. Such analyses predict the existence of nonpointlike, dynamical quark-quark (diquark) correlations within all baryons; and a uniformly sound description of the systems studied is obtained by retaining flavor-antitriplet-scalar and flavor-sextet-pseudovector diquarks. Thus constituted, the rest-frame wave function of every system studied is primarily S wave in character; and the fast positive-parity excitation of each octet or decuplet baryon exhibits the characteristics of a radial excitation. Importantly, every ground-state octet and decuplet baryon possesses a radial excitation. Hence, the analysis predicts the existence and masses of positive-parity excitations of the Ξ, Ξ*, and Ω baryons, states which have not yet been empirically identified. This body of analysis suggests that the expression of emergent mass generation is the same in all u , d , and s baryons and, notably, that dynamical quark-quark correlations play an essential role in the structure of each one. Furthermore, it also provides the basis for developing an array of predictions that can be tested in new generation experiments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Spectroscopic Studies on the Metal-Insulator Transition Mechanism in Correlated Materials

Here, the metal–insulator transition (MIT) in correlated materials is a novel phenomenon that accompanies a large change in resistivity, often many orders of magnitude. It is important in its own right but its switching behavior in resistivity can be useful for device applications. From the material physics point of view, the starting point of the research on the MIT should be to understand the microscopic mechanism. Here, an overview of recent efforts to unravel the microscopic mechanisms for various types of MITs in correlated materials is provided. Research has focused on transition metal oxides (TMOs), but transition metal chalcogenides have also been studied. Along the way, a new class of MIT materials is discovered, the so–called relativistic Mott insulators in 5d TMOs. Distortions in the MO 6 (M = transition metal) octahedron are found to have a large and peculiar effect on the band structure in an orbital dependent way, possibly paving a way to the orbital selective Mott transition. In the final section, the character of the materials suitable for applications is summarized, followed by a brief discussion of some of the efforts to control MITs in correlated materials, including a dynamical approach using light.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Dynamics of fractionalized mean-field theories: Consequences for Kitaev materials

There have been substantial recent efforts, both experimentally and theoretically, to find a material realization of the Kitaev spin liquid—the ground state of the exactly solvable Kitaev model on the honeycomb lattice. Candidate materials are now plentiful, but the presence of non-Kitaev terms makes comparison between theory and experiment challenging. Here, we rederive time-dependent Majorana mean-field theory and extend it to include quantum phase information, allowing the direct computation of the experimentally relevant dynamical spin-spin correlator, which reproduces exact results for the unperturbed model. In contrast to previous work, we find that small perturbations do not substantially alter the exact result, implying that α-RuCl 3 is perhaps farther from the Kitaev phase than originally thought. Our approach generalizes to any correlator and to any model where Majorana mean-field theory is a valid starting point.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Optical spectra in the condensed phase: Capturing anharmonic and vibronic features using dynamic and static approaches

Simulating optical spectra in the condensed phase remains a challenge for theory due to the need to capture spectral signatures arising from anharmonicity and dynamical effects, such as vibronic progressions and their induced asymmetry. As such, numerous simulation methods have been developed that invoke different approximations and vary in their ability to capture different physical regimes. In this work, we use several models of chromophores in the condensed phase and ab initio molecular dynamics simulations to rigorously assess the applicability of methods to simulate optical absorption spectra. Specifically, we focus on the ensemble scheme, which can address anharmonic potential energy surfaces but relies on the applicability of extreme nuclear-electronic timescale separation; the Franck-Condon method, which includes dynamical effects but only at the harmonic level; as well as the recently introduced ensemble zero-temperature Franck-Condon approach, which straddles these limits. We also devote particular attention to the performance of methods derived from a cumulant expansion of the energy gap fluctuations and test the ability to approximate the requisite time correlation functions using classical dynamics with quantum correction factors. These results provide insights as to when these methods are applicable and able to capture the features of condensed phase spectra qualitatively and, in some cases, quantitatively across a range of regimes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

STEADY-STATE RELATIVISTIC STELLAR DYNAMICS AROUND A MASSIVE BLACK HOLE

A massive black hole (MBH) consumes stars whose orbits evolve into the small phase-space volume of unstable orbits, the “loss cone,” which take them into the MBH, or close enough to interact strongly with it. The resulting phenomena, e.g., tidal heating and disruption, binary capture and hyper-velocity star ejection, gravitational wave (GW) emission by inspiraling compact remnants, or hydrodynamical interactions with an accretion disk, can produce observable signatures and thereby reveal the MBH, affect its mass and spin evolution, test strong gravity, and probe stars and gas near the MBH. These continuous stellar loss and resupply processes shape the central stellar distribution. We investigate relativistic stellar dynamics near the loss cone of a non-spinning MBH in steady state, analytically and by Monte Carlo simulations of the diffusion of the orbital parameters. These take into account Newtonian mass precession due to enclosed stellar mass, in-plane precession due to general relativity, dissipation by GW, uncorrelated two-body relaxation, correlated resonant relaxation (RR), and adiabatic invariance due to secular precession, using a rigorously derived description of correlated post-Newtonian dynamics in the diffusion limit. We argue that general maximal entropy considerations strongly constrain the orbital diffusion in steady state, irrespective of the relaxation mechanism. We identify the exact phase-space separatrix between plunges and inspirals, and predict their steady-state rates. We derive the dependence of the rates on the mass of the MBH, show that the contribution of RR in steady state is small, and discuss special cases where unquenched RR in restricted volumes of phase-space may affect the steady state substantially.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Functional renormalization-group approaches, one-particle (irreducible) reducible with respect to local Green’s functions, with dynamical mean-field theory as a starting point

We consider formulations of the functional renormalization-group (fRG) flow for correlated electronic systems with the dynamical mean-field theory as a starting point. We classify the corresponding renormalization-group schemes into those neglecting one-particle irreducible six-point vertices (with respect to the local Green’s functions) and neglecting one-particle reducible six-point vertices. The former class is represented by the recently introduced DMF{sup 2}RG approach [31], but also by the scale-dependent generalization of the one-particle irreducible representation (with respect to local Green’s functions, 1PI-LGF) of the generating functional [20]. The second class is represented by the fRG flow within the dual fermion approach [16, 32]. We compare formulations of the fRG approach in each of these cases and suggest their further application to study 2D systems within the Hubbard model.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Sub-system quantum dynamics using coupled cluster downfolding techniques

In this paper, we discuss extending the sub-system embedding sub-algebra coupled cluster (SES-CC) formalism and the double unitary coupled cluster (DUCC) ansatz to the time domain. As we demonstrated in earlier studies, it is possible, using these formalisms, to calculate the energy of the entire system as an eigenvalue of downfolded/effective Hamiltonian in the active space, that is identifiable with the sub-system of the composite system. In these studies, we demonstrated that downfolded Hamiltonians integrate out Fermionic degrees of freedom that do not correspond to the physics encapsulated by the active space. We extend these results to the time-dependent Schrödinger equation, showing that a similar construct is possible to partition a system into a sub-system that varies slowly in time and a remaining subsystem that corresponds to fast oscillations. This time dependent formalism allows coupled cluster quantum dynamics to be extended to larger systems and for the formulation of novel quantum algorithms based on the quantum Lanczos approach, which have recently been considered in the literature.

coupled cluster, Electron correlation, quantum dyn↗
DOE OSTI2023

Scrambling and operator entanglement in local non-Hermitian quantum systems

The breakdown of Lieb-Robinson bounds in local, non-Hermitian quantum systems opens up the possibility for a rich landscape of quantum many-body phenomenology. We elucidate this by studying information scrambling and quantum chaos in non-Hermitian variants of paradigmatic local quantum spin-chain models. We utilize a mixture of exact diagonalization and tensor network techniques for our numerical results and focus on three dynamical quantities: (i) out-of-time-ordered correlators (OTOCs), (ii) operator entanglement of the dynamics, and (iii) entanglement growth following a quench from product initial states. We show that while OTOCs fail to capture information scrambling in a simple, local, non-Hermitian transverse-field Ising model, the closely related operator entanglement is a robust measure of dynamical properties of interest. Moreover, we show that the short-time growth of operator entanglement can generically detect entanglement phase transitions in these systems while its long-time average is shown to be a reliable indicator of quantum chaos and entanglement phases. This allows us to extend operator entanglement-based diagnostics from previous works on closed and open quantum systems, to the new arena of monitored quantum dynamics. Finally, we remark on the efficacy of these dynamical quantities in detecting integrability/chaos in the presence of continuous monitoring.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Experimental Study of TCP Throughput Profiles and Dynamics Over Dedicated Connections

A throughput profile expressed as a function of the round-trip times of a data transport infrastructure is a critical indicator of its level of optimization, particularly, over dedicated connections. We study the throughput profiles of eleven TCP versions using measurements collected over dedicated hardware-emulated connections with distances spanning round the earth. Among them, BBR has overall higher temporal variations and lower throughput profiles compared to five loss-based TCP versions, and the comparison with other TCP versions is mixed. Using the Poincare map regions of throughput time traces, we show that the richer dynamics of BBR are correlated with its lower throughput profiles. We present basic analytical results that indicate that higher temporal variations of TCP methods lead to lower throughput profiles, thereby establishing the underlying causality. Under external losses, BBR achieves sustained high throughput compared to others as the loss rate is increased. Overall, our results provide insights into the relationship between time dynamics and throughput profiles of TCP versions, in particular, show that limited time traces can be indicative of global properties of throughput profiles.

Rao, Nageswara↗
DOE OSTI2023

Structure, Dynamics, and Hydrogen Transport in Amorphous Polymers: An Analysis of the Interplay between Free Volume Element Distribution and Local Segmental Dynamics from Molecular Dynamics Simulations

Polymers are attractive membrane materials owing to their mechanical robustness and relatively inexpensive fabrication. An important indicator of membrane performance are free volume elements (FVE): microporous void spaces created by the inefficient packing of bulky groups along the polymer chain. FVEs tend to degrade over time, as polymer chains reorganize irreversibly. While it is widely accepted that polymer flexibility has an impact on membrane transport properties, the molecular nature of this impact is still not well understood. By the establishment of a correlation between local chain dynamics and the distribution of free volume elements (FVEs), penetrant transport can be regulated more efficiently in amorphous polymer membranes. In this work, we implement all-atom molecular dynamics (MD) simulations to explore the relationship between chain dynamics and free volume in three polymers with different levels of backbone flexibility: polymethylpentene (PMP), polystyrene (PS), and HAB-6FDA thermally rearranged polymer (TRP). We construct these polymers at different temperatures and examine how temperature impacts the FVE distribution and segmental mobility. Our analysis shows that chain segments near FVEs have higher mobility compared with the atoms in the bulk; the extent of this difference increases with chain flexibility. Increasing the chain flexibility by increasing the temperature results in a broader FVE distribution. Rigid polymers such as TRP show the most robust FVE distribution and are not significantly affected by the temperature change. To capture penetrant diffusion through the polymer matrix, hydrogen is inserted and the diffusion is measured at different temperatures; hydrogen mobility is influenced by the FVE structure and overall mobility of polymer chains. Lastly, at low temperatures, hydrogen mobility is influenced by void distribution, while at high temperatures, polymer dynamics dictate hydrogen transport.

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

Deep learning with plasma plume image sequences for anomaly detection and prediction of growth kinetics during pulsed laser deposition

Abstract Materials synthesis platforms that are designed for autonomous experimentation are capable of collecting multimodal diagnostic data that can be utilized for feedback to optimize material properties. Pulsed laser deposition (PLD) is emerging as a viable autonomous synthesis tool, and so the need arises to develop machine learning (ML) techniques that are capable of extracting information from in situ diagnostics. Here, we demonstrate that intensified-CCD image sequences of the plasma plume generated during PLD can be used for anomaly detection and the prediction of thin film growth kinetics. We develop multi-output (2 + 1)D convolutional neural network regression models that extract deep features from plume dynamics that not only correlate with the measured chamber pressure and incident laser energy, but more importantly, predict parameters of an auto-catalytic film growth model derived from in situ laser reflectivity experiments. Our results demonstrate how ML with in situ plume diagnostics data in PLD can be utilized to maintain deposition conditions in an optimal regime. Further, the predictive capabilities of plume dynamics on the kinetics of film growth or other film properties prior to deposition provides a means for rapid pre-screening of growth conditions for the non-expert, which promises to accelerate materials optimization with PLD.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Electronic correlation induced expansion of Fermi pockets in δ-plutonium

Plutonium is a critically important material as the behavior of its 5f electrons stands midway between the metalliclike itinerant character of the light actinides and localized atomic-core-like character of the heavy actinides. The δ phase of plutonium (δ-Pu), whereas still itinerant, has a large coherent Kondo peak and strong electronic correlations coming from its near-localized character. Here, using sophisticated Gutzwiller wave function and dynamical mean-field theory correlated theories, we study the Fermi surface and associated mass renormalizations of δ-Pu together with calculations of the de Haas–van Alphen frequencies. We find a large (~200%) correlation induced volume expansion in both the hole and the electron pockets of the Fermi surface in addition to an intermediate mass enhancement. All of the correlated electron theories predict, approximately, the same hole pocket placement in the Brillouin zone, which is different from that obtained in conventional density-functional band-structure theory, whereas the electron pockets from all theories are in, roughly, the same place.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1977

Differential altimetry for satellite orbit determination

Differential altimetry is concerned with the employment of differenced satellite altimeter measurements at orbit ground trace intersections. The employment of this procedure makes it possible to eliminate two of the major error sources found in direct altimetry. Previous applications have not included the appropriate dynamic constraints required to account for correlations due to satellite orbit motion. A description is given of an investigation in which these correlations are included. The methodology produced is consistent with the dynamic environment. The regional or local limitations of previous approaches are overcome by extending the technique to the global scale. Attention is given to the description of the data type, the geometric topography height, altimeter errors, discretization errors, an approximate orbit determination problem, and a comparison of differenced altimeter measurements for retrograde and prograde orbits.

Hagar, H., Jr.↗
NASA NTRS1982

The distant interplanetary wake of Venus - Plasma observations from Pioneer Venus

Observations by the Pioneer Vernus Orbiter plasma analyzer during passages through the Venus solar wind wake in June 1979 are reported. The spacecraft traveled 8-12 Venus radii behind the planet from the sun, detecting frequent, episodic disappearances of the plasma. The disappearance occurred inside the magnetotail, indicating a tattered, filamentary extension of the solar wind cavity. Positive oxygen ions were observed inside and outside of the magnetotail on some days, and were absent on others. The data indicate that the cavity contracts during high solar wind dynamic pressure, although the presence of 0(+) ions is not correlated well with the solar wind dynamic pressure. The most intense bursts originated from a flux of 10 million ions/sq cm per sec, with an 0(+) kinetic energy estimated to be 100,000-1,000,000 K.

Mihalov, J. D.↗
DOE OSTI2021

Statistical Correlation Between Quantum Entanglement and Spin–Orbit Coupling in Crossed Beam Molecular Dynamics

Non-classical features like interference are already being harnessed to control the output of chemical reactions. However, quantum entanglement which is an equally enigmatic many-body quantum correlation can also be used as a powerful resource yet has eluded explicit attention. In this report, an experimental scheme under the crossed beam molecular dynamical setup, with the F + HD reaction, is proposed aiming to study the possible influence of entanglement within reactant pairs on the angular features of the product distribution. The aforesaid reaction has garnered interest recently, as an unusual horseshoe shape pattern in the product (HF) distribution was observed, which has been attributed to the coupling of spin and orbital degrees of freedom. An experimental scheme is proposed aiming to study the possible influence of entanglement on the necessity for the inclusion of such spin–orbit characteristics, under circumstances wherein the existence of entanglement and spin–orbit interaction is simultaneously detectable. The attainable results are further numerically simulated highlighting specific patterns corresponding to various possibilities. Finally, such studies if extended can provide unforeseen mechanistic insight into analogous reactions, too, from the lens of quantum information.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗