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At least 1,261 records · Page 70

Transport properties of nanocomposite and its simulation with L-R-C circuit

The nano particles are represented in this communication by L-R-C equivalent circuit. The dc current voltage characteristics (CVC) of the proposed circuit have simulated using Circuit-Maker ® 2000. Experimental investigation on ZnO nano-composite with capping material gum acacia shows similar CVC. NPs are represented by C-R combinations to manifest the Coulomb blockade effect of a quantum dot. The capping material is represented by an inductor along with a resistance in series. Nine NPs with capping matrix are simulated. The dc current voltage characteristics (CVC) and gross feature of polarization nature obtained by experiment and simulation study are consistent.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

The Prelle-Singer method and Painlevé hierarchies

We consider systems of ordinary differential equations (ODEs) of the form BK=0, where B is a Hamiltonian operator of a completely integrable partial differential equation hierarchy, and K = (K, L){sup T}. Such systems, while of quite low order and linear in the components of K, may represent higher-order nonlinear systems if we make a choice of K in terms of the coefficient functions of B. Indeed, our original motivation for the study of such systems was their appearance in the study of Painlevé hierarchies, where the question of the reduction of order is of great importance. However, here we do not consider such particular cases; instead we study such systems for arbitrary K, where they may represent both integrable and nonintegrable systems of ordinary differential equations. We consider the application of the Prelle-Singer (PS) method—a method used to find first integrals—to such systems in order to reduce their order. We consider the cases of coupled second order ODEs and coupled third order ODEs, as well as the special case of a scalar third order ODE; for the case of coupled third order ODEs, the development of the PS method presented here is new. We apply the PS method to examples of such systems, based on dispersive water wave, Ito and Korteweg-de Vries Hamiltonian structures, and show that first integrals can be obtained. It is important to remember that the equations in question may represent sequences of systems of increasing order. We thus see that the PS method is a further technique which we expect to be useful in our future work.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High-density carbon ablator experiments on the National Ignition Facility

High Density Carbon (HDC) is a leading candidate as an ablator material for Inertial Confinement Fusion (ICF) capsules in x-ray (indirect) drive implosions. HDC has a higher density (3.5 g/cc) than plastic (CH, 1 g/cc), which results in a thinner ablator with a larger inner radius for a given capsule scale. This leads to higher x-ray absorption and shorter laser pulses compared to equivalent CH designs. This paper will describe a series of experiments carried out to examine the feasibility of using HDC as an ablator using both gas filled hohlraums and lower density, near vacuum hohlraums. These experiments have shown that deuterium (DD) and deuterium-tritium gas filled HDC capsules driven by a hohlraum filled with 1.2 mg/cc He gas, produce neutron yields a factor of 2× higher than equivalent CH implosions, representing better than 50% Yield-over-Clean (YoC). In a near vacuum hohlraum (He = 0.03 mg/cc) with 98% laser-to-hohlraum coupling, such a DD gas-filled capsule performed near 1D expectations. A cryogenic layered implosion version was consistent with a fuel velocity = 410 ± 20 km/s with no observed ablator mixing into the hot spot.

01 COAL, LIGNITE, AND PEAT↗

Sequence stratigraphy of the Miocene, Pohokura field, Taranaki Basin, New Zealand

A sequence stratigraphic study of the Miocene age was conducted in the Pohokura field, that is located offshore from the northern coast of Taranaki Penisula, New Zealand. It is a low-relief, north-south elongated anticline approximately 16 km long and 5 km wide. The study was carried out with two objectives which are to identify the Miocene seismic facies and to identify the sequence stratigraphic parameters. One seismic line and Pohokura-2 well was use in the study. Various seismic facies were observed in the seismic section including parallel, subparallel, continuous, subcontinuous, wavy, free reflection, subchaotic, high amplitude-high frequency and high amplitude-low frequency reflection. The interpreted seismic line showed three chronostratigraphic units which is sequence boundary 1 (SB1) represent top Manganui, sequence boundary 2 (SB2) represent top Mount Messenger and sequence boundary 3 (SB3) represent top Urenui. SB1, was separated by two distinct seismic facies namely sub-parallel and sub-chaotic. Parallel and sub-parallel reflection was observed on top of the sequence boundary SB2 while sub-chaotic and wavy seismic facies is found below the sequence boundary. SB3 is characterize by erosional truncation as shown by the present of toplap and downlap terminations in the western part of the seismic section. It is also supported by the clear difference of very high amplitud-high frequency reflection on top of SB3 overlying low amplitud-low frequency reflection of Urenui Formation. A complete depositional system including highstand, lowstand and transgressive system tracts are observed in the incised valley within the Urenui Formation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Potential energy surfaces for the HBr{sup +} + CO{sub 2} → Br + HOCO{sup +} reaction in the HBr{sup +} {sup 2}Π{sub 3/2} and {sup 2}Π{sub 1/2} spin-orbit states

Quantum mechanical (QM) + molecular mechanics (MM) models are developed to represent potential energy surfaces (PESs) for the HBr{sup +} + CO{sub 2} → Br + HOCO{sup +} reaction with HBr{sup +} in the {sup 2}Π{sub 3/2} and {sup 2}Π{sub 1/2} spin-orbit states. The QM component is the spin-free PES and spin-orbit coupling for each state is represented by a MM-like analytic potential fit to spin-orbit electronic structure calculations. Coupled-cluster single double and perturbative triple excitation (CCSD(T)) calculations are performed to obtain “benchmark” reaction energies without spin-orbit coupling. With zero-point energies removed, the “experimental” reaction energy is 44 ± 5 meV for HBr{sup +}({sup 2}Π{sub 3/2}) + CO{sub 2} → Br({sup 2}P{sub 3/2}) + HOCO{sup +}, while the CCSD(T) value with spin-orbit effects included is 87 meV. Electronic structure calculations were performed to determine properties of the BrHOCO{sup +} reaction intermediate and [HBr⋯OCO]{sup +} van der Waals intermediate. The results of different electronic structure methods were compared with those obtained with CCSD(T), and UMP2/cc-pVTZ/PP was found to be a practical and accurate QM method to use in QM/MM direct dynamics simulations. The spin-orbit coupling calculations show that the spin-free QM PES gives a quite good representation of the shape of the PES originated by {sup 2}Π{sub 3/2}HBr{sup +}. This is also the case for the reactant region of the PES for {sup 2}Π{sub 1/2} HBr{sup +}, but spin-orbit coupling effects are important for the exit-channel region of this PES. A MM model was developed to represent these effects, which were combined with the spin-free QM PES.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Communication: Fully coherent quantum state hopping

In this paper, we describe a new and fully coherent stochastic surface hopping method for simulating mixed quantum-classical systems. We illustrate the approach on the simple but unforgiving problem of quantum evolution of a two-state quantum system in the limit of unperturbed pure state dynamics and for dissipative evolution in the presence of both stationary and nonstationary random environments. We formulate our approach in the Liouville representation and describe the density matrix elements by ensembles of trajectories. Population dynamics are represented by stochastic surface hops for trajectories representing diagonal density matrix elements. These are combined with an unconventional coherent stochastic hopping algorithm for trajectories representing off-diagonal quantum coherences. The latter generalizes the binary (0,1) “probability” of a trajectory to be associated with a given state to allow integers that can be negative or greater than unity in magnitude. Unlike existing surface hopping methods, the dynamics of the ensembles are fully entangled, correctly capturing the coherent and nonlocal structure of quantum mechanics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Feynman formulae and phase space Feynman path integrals for tau-quantization of some Lévy-Khintchine type Hamilton functions

Evolution semigroups generated by pseudo-differential operators are considered. These operators are obtained by different (parameterized by a number τ) procedures of quantization from a certain class of functions (or symbols) defined on the phase space. This class contains Hamilton functions of particles with variable mass in magnetic and potential fields and more general symbols given by the Lévy-Khintchine formula. The considered semigroups are represented as limits of n-fold iterated integrals when n tends to infinity. Such representations are called Feynman formulae. Some of these representations are constructed with the help of another pseudo-differential operator, obtained by the same procedure of quantization; such representations are called Hamiltonian Feynman formulae. Some representations are based on integral operators with elementary kernels; these are called Lagrangian Feynman formulae. Langrangian Feynman formulae provide approximations of evolution semigroups, suitable for direct computations and numerical modeling of the corresponding dynamics. Hamiltonian Feynman formulae allow to represent the considered semigroups by means of Feynman path integrals. In the article, a family of phase space Feynman pseudomeasures corresponding to different procedures of quantization is introduced. The considered evolution semigroups are represented as phase space Feynman path integrals with respect to these Feynman pseudomeasures, i.e., different quantizations correspond to Feynman path integrals with the same integrand but with respect to different pseudomeasures. This answers Berezin’s problem of distinguishing a procedure of quantization on the language of Feynman path integrals. Moreover, the obtained Lagrangian Feynman formulae allow also to calculate these phase space Feynman path integrals and to connect them with some functional integrals with respect to probability measures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Energy landscapes and persistent minima

We consider a coarse-graining of high-dimensional potential energy landscapes based upon persistences, which correspond to lowest barrier heights to lower-energy minima. Persistences can be calculated efficiently for local minima in kinetic transition networks that are based on stationary points of the prevailing energy landscape. The networks studied here represent peptides, proteins, nucleic acids, an atomic cluster, and a glassy system. Minima with high persistence values are likely to represent some form of alternative structural morphology, which, if appreciably populated at the prevailing temperature, could compete with the global minimum (defined as infinitely persistent). Threshold values on persistences (and in some cases equilibrium occupation probabilities) have therefore been used in this work to select subsets of minima, which were then analysed to see how well they can represent features of the full network. Simplified disconnectivity graphs showing only the selected minima can convey the funnelling (including any multiple-funnel) characteristics of the corresponding full graphs. The effect of the choice of persistence threshold on the reduced disconnectivity graphs was considered for a system with a hierarchical, glassy landscape. Sets of persistent minima were also found to be useful in comparing networks for the same system sampled under different conditions, using minimum oriented spanning forests.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing surface recombination velocities in semiconductors using two-photon microscopy

The determination of minority-carrier lifetimes and surface recombination velocities is essential for the development of semiconductor technologies such as solar cells. The recent development of two-photon time-resolved microscopy allows for better measurements of bulk and subsurface interfaces properties. Here, we analyze the diffusion problem related to this optical technique. Our three-dimensional treatment enables us to separate lifetime (recombination) from transport effects (diffusion) in the photoluminescence intensity. It also allows us to consider surface recombination occurring at a variety of geometries: a single plane (representing an isolated exposed or buried interface), a two parallel planes (representing two inequivalent interfaces), and a spherical surface (representing the enclosing surface of a grain boundary). We provide fully analytical results and scalings directly amenable to data fitting and apply those to experimental data collected on heteroepitaxial CdTe/ZnTe/Si.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Permutation invariant polynomial neural network approach to fitting potential energy surfaces. IV. Coupled diabatic potential energy matrices

A machine learning method is proposed for representing the elements of diabatic potential energy matrices (PEMs) with high fidelity. This is an extension of the so-called permutation invariant polynomial-neural network (PIP-NN) method for representing adiabatic potential energy surfaces. While for one-dimensional irreducible representations the diagonal elements of a diabatic PEM are invariant under exchange of identical nuclei in a molecular system, the off-diagonal elements require special symmetry consideration, particularly in the presence of a conical intersection. A multiplicative factor is introduced to take into consideration the particular symmetry properties while maintaining the PIP-NN framework. Here, we demonstrate here that the extended PIP-NN approach is accurate in representing diabatic PEMs, as evidenced by small fitting errors and by the reproduction of absorption spectra and product branching ratios in both H 2 O$(\tilde{X} / \tilde{B})$ and NH 3 $(\tilde{X} $/Ã) non-adiabatic photodissociation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Pressure-induced polymorphism and piezochromism in Mn 2 FeSbO 6

In the last decade, major efforts have been devoted to searching for polar magnets due to their vast potential applications in spintronic devices. However, the polar magnets are rare because of conflicting electronic configuration requirements of ferromagnetism and electric polarization. Double-perovskite oxides with a polar structure containing transition metal elements represent excellent candidates for the polar magnet design. In this work, the crystal structure evolution of Mn 2 FeSbO 6 (MFSO) was investigated at pressures reaching ~50 GPa by in situ synchrotron X-ray diffraction (XRD), Raman scattering, and ab initio calculation techniques. The XRD results reveal ilmenite- to perovskite-type phase transition at around 35 GPa. An additional intermediate phase, observed in the range of 31–36 GPa by Raman spectroscopy, but not the XRD technique, is proposed to represent the polar LiNbO 3 phase. It is argued that this phase emerged due to the heating effect of the Raman-excitation laser. The LiNbO 3 -type MFSO compounds, displaying an intrinsic dipole ordering, represent a promising candidate for multiferroic materials. The detected phase transitions were found to be reversible although a significant hysteresis was noticeable between compression and decompression runs. Moreover, a pressure-induced piezochromism, signifying a bandgap change, was discovered by the direct visual observations and corroborated by ab initio calculations. The present study benefits an efficient high-pressure synthesis of polar magnetic double-perovskite oxides in the future.

36 MATERIALS SCIENCE↗

Causal interaction in high frequency turbulence at the biosphere–atmosphere interface: Structural behavior

High-frequency (e.g., 10 Hz) eddy covariance measurements are typically used to estimate fluxes at the land–atmosphere interface at timescales of 15–60 min. These multivariate data contain information about the interdependency at high frequency between the interacting variables such as wind, humidity, temperature, and CO 2⁠ . We use data at 10 Hz from an eddy covariance instrument located at 25 m above agricultural land in the Midwestern US, which offers an opportunity to move beyond the traditional spectral analyses to explore causal dependency among variables. In this study, we quantify the structure of inter-dependencies of interacting variables at high frequency represented by a directed acyclic graph (DAG). We compare DAGs to investigate changes in structural differences in causal interactions. We then apply a distance-based classification and -means clustering approach to identify the evolution of the causal structure represented by a DAG. Our method selects an unbiased number of clusters of similar structures and characterizes the similarities and differences between them. We explore a range of dynamic behavior using data from a clear sky day and during a solar eclipse in 2017. Our results show well-defined clusters of similar causal dependencies as the system evolves. Furthermore, our approach provides a methodological framework to understand how causal dependence in turbulence manifests in high-frequency data when represented through a DAG.

54 ENVIRONMENTAL SCIENCES↗

Elucidating ion capture and transport mechanisms of Preyssler anions in aqueous solutions using biased MACE-accelerated MD simulations

Equilibrium and biased multi-atomic cluster expansion (MACE) accelerated molecular dynamics (MD) simulations in aqueous solutions are performed to investigate the ion capture and transport mechanisms of the {P 5 W 30 } Preyssler anion (PA) as the smallest representative member of the extended polyoxometalate (POM) family with an internal cavity. The unique interatomic interactions present in the internal cavity vs the exterior of PA are carefully investigated using equilibrium MACE MD simulations for two representative Na(H 2 O)@PA and Na@PA complexes in aqueous solutions. Our careful analyses of radial distribution functions and coordination numbers show that the presence of confined water in Na(H 2 O)@PA has profound modulating effects on the nature of the interactions of the encapsulated ion with the oxygens of the PA cavity. Using well-converged MACE-accelerated multiple walker well-tempered metadynamics simulations with nanosecond timescales, two different associative (ion exchange) and dissociative (ion ejection) ion transport mechanisms were carefully investigated for Na + as one of the most abundant and representative ions present in seawater and saline solutions. By comparing systems with and without confined water, it was found that the presence of only one pre-encapsulated confined water in Na(H 2 O)@PA dramatically changes the free energy landscape of ion transport processes. It was also found that the contraction and dilation of the two windows present in PA directly influence the Na + and H 2 O transport. Furthermore, the results from this work are helpful, as they show a viable path toward tuning the ion exchange and transport phenomena in aqueous solutions of POM molecular clusters and frameworks.

25 ENERGY STORAGE↗

Locally purified maximally mixed states at scale: Entanglement pruning and symmetries

Locally Purified Density Operators (LPDOs) are state-of-the-art tensor network ansatze candidates that efficiently represent mixed quantum states at scale. However, given their non-uniqueness, their representational complexity is generally sub-optimal in practical computations. Here, in this work we perform a comprehensive numerical and analytical analysis and resolve this issue in the experimentally relevant limit where noise depolarizes the density operator into a maximally mixed state. To resolve the sub-optimality issue, we analyze two numerical tools, one analytic method, and detail the relations between them. The numerical tools used are fidelity-preserving truncations and isometric gauge transformations leveraging Riemannian optimizations over entropic objective functions. In addition, by invoking the injectivity and symmetry constraints of the maximally mixed LPDO, we also present analytical closed-form expressions for the disentangler and discuss their relation to numerical optimizers. Further, away from the maximally mixed state, our simulations highlight how the truncation threshold smoothly interpolate, as a function of depolarization, between established matrix product results and our new results. Our work shows how, by minimizing the resources required to represent key states of practical interest in experiment, the efficiency of tensor network algorithms can be substantially increased. This paves the path for uncovering tensor network’s fundamental scalability limits and latent potential in representing the wide locus of mixed quantum states that are accessible on near-term quantum devices.

Gangapuram, Amit Jamadagni [Oak Ridge National Lab↗

On the universal structure of human lexical semantics

How universal is human conceptual structure? The way concepts are organized in the human brain may reflect distinct features of cultural, historical, and environmental background in addition to properties universal to human cognition. Semantics, or meaning expressed through language, provides indirect access to the underlying conceptual structure, but meaning is notoriously difficult to measure, let alone parameterize. Here, we provide an empirical measure of semantic proximity between concepts using cross-linguistic dictionaries to translate words to and from languages carefully selected to be representative of worldwide diversity. These translations reveal cases where a particular language uses a single “polysemous” word to express multiple concepts that another language represents using distinct words. We use the frequency of such polysemies linking two concepts as a measure of their semantic proximity and represent the pattern of these linkages by a weighted network. This network is highly structured: Certain concepts are far more prone to polysemy than others, and naturally interpretable clusters of closely related concepts emerge. Statistical analysis of the polysemies observed in a subset of the basic vocabulary shows that these structural properties are consistent across different language groups, and largely independent of geography, environment, and the presence or absence of a literary tradition. As a result, the methods developed here can be applied to any semantic domain to reveal the extent to which its conceptual structure is, similarly, a universal attribute of human cognition and language use.

96 KNOWLEDGE MANAGEMENT AND PRESERVATION↗

Illuminating structural proteins in viral "dark matter" with metaproteomics

Viruses are ecologically important, yet environmental virology is limited by dominance of unannotated genomic sequences representing taxonomic and functional "viral dark matter." Although recent analytical advances are rapidly improving taxonomic annotations, identifying functional darkmatter remains problematic. Here, we apply paired metaproteomics and dsDNA-targeted metagenomics to identify 1,875 virion-associated proteins from the ocean. Over one-half of these proteins were newly functionally annotated and represent abundant and widespread viral metagenome-derived protein clusters (PCs). One primarily unannotated PC dominated the dataset, but structural modeling and genomic context identified this PC as a previously unidentified capsid protein from multiple uncultivated tailed virus families. Furthermore, four of the five most abundant PCs in the metaproteome represent capsid proteins containing the HK97-like protein fold previously found in many viruses that infect all three domains of life. The dominance of these proteins within our dataset, as well as their global distribution throughout the world's oceans and seas, supports prior hypotheses that this HK97-like protein fold is the most abundant biological structure on Earth. Altogether, these culture-independent analyses improve virion-associated protein annotations, facilitate the investigation of proteins within natural viral communities, and offer a high-throughput means of illuminating functional viral dark matter.

59 BASIC BIOLOGICAL SCIENCES↗

Lability of secondary organic particulate matter

Accurate simulations of the consenctrations of atmospheric organic particulate matter (PM) are needed for predicting energy flow in the Earth’s climate system. In the past, simulations of organic PM widely assume equilibrium partitioning of semivolatile organic compounds (SVOCs) between the PM and surrounding vapor. Herein, we test this assumption by measuring evaporation rates and associated vapor mass concentration of organic films representative of atmospheric PM. For films representing anthropogenic PM, evaporation rates and vapor mass concentrations increased above a threshold relative humidity (RH), indicating equilibrium partitioning above a transition RH but not below. In contrast for films representing biogenic PM, no threshold was observed, indicating equilibrium partitioning at all RHs. The results suggest that the mass lability of atmospheric organic PM can differ in consequential ways among Earth’s natural biomes, polluted regions, and regions of land-use change, and these differences need to be considered when simulating atmospheric organic PM.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-dependent water dynamics in hydrated uranyl fluoride

In this study, uranyl fluoride is a three-layer, hexagonal structure with significant stacking disorder in the c-direction. It supports a range of unsolved ‘thermodynamic’ hydrates with 0–2.5 water molecules per uranium atom, and perhaps more. However, the relationship between water, hydrate crystal structures, and thermodynamic results, collectively representing the chemical pathway through these hydrate structures, has not been sufficiently elucidated. We used high-resolution quasielastic neutron scattering to study the dynamics of water in partially hydrated uranyl fluoride powder over the course of 4 weeks under closed conditions. The spectra are composed of two quasielastic components: one is associated with translational diffusive motion of water that is approximately five to six times slower than bulk water, and the other is a slow (on the order of 2–300 ps), spatially bounded water motion. The translational component represents water diffusing between the weakly bonded layers in the crystal, while the bounded component may represent water trapped in subnanometre ‘pockets’ formed by the space between uranium-centred polymerisation units. Complementary neutron diffraction measurements do not show any significant structural changes, suggesting that a chemical conversion of the material does not occur in the thermodynamically isolated system on this timescale.

36 MATERIALS SCIENCE↗