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At least 127 records · Page 7

Dynamic decay of a single vortex into vortex-antivortex pairs

A variety of metastable states, including vortices, antivortices, and their combinations, is typical for magnetically soft, thin films and patterned structures. The physics of individual spin vortices in patterned structures has been rather extensively explored. In contrast, there are few studies of the vortex–antivortex–vortex (v-av-v) system, in part because the configuration is rather challenging to obtain experimentally. We demonstrate herein how a recently proposed resonant-spin-ordering technique can be used to induce the dynamic decay of a single vortex into v-av states in elongated elements. The approach is based on first driving the system from the linear regime of constant vortex gyrations to the non-linear regime of vortex-core reversals at a fixed excitation frequency, and then subsequently reducing the excitation field back to the linear regime. This procedure stabilizes the system into a v-av-v state that is completely decoupled from the initialization excitation frequency. The newly acquired state is stable in remanence. The dynamic response of this system is expected to demonstrate a number of collective modes, depending on the combination of the vortex core polarities, and/or the excitation field direction, and, hence, is of interest for future studies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

{pi} junction and spontaneous current state in a superfluid Fermi gas

We discuss an idea to realize a spontaneous current in a superfluid Fermi gas. When a polarized Fermi superfluid (N{sub {up_arrow}}>N{sub {down_arrow}}, where N{sub {sigma}} is the number of atoms in the hyperfine state described by pseudospin {sigma}={up_arrow},{down_arrow}) is loaded onto a ring-shaped trap with a weak potential barrier, some excess atoms ({Delta}N=N{sub {up_arrow}}-N{sub {down_arrow}}) are localized around the barrier. As shown in our previous paper [T. Kashimura, S. Tsuchiya, and Y. Ohashi, Phys. Rev. A 82, 033617 (2010)], this polarized potential barrier works as a {pi} junction in the sense that the superfluid order parameter changes its sign across the barrier. Because of this, the phase of the superfluid order parameter outside the junction is shown to be twisted by {pi} along the ring, which naturally leads to a circulating supercurrent. While the ordinary supercurrent state is obtained as a metastable state, this spontaneous current state is shown to be more stable than the case with no current. Our results indicate that localized excess atoms would be useful for the manipulation of the superfluid order parameter in cold Fermi gases.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Selective formation of metastable polymorphs in solid-state synthesis

Metastable polymorphs often result from the interplay between thermodynamics and kinetics. Despite advances in predictive synthesis for solution-based techniques, there remains a lack of methods to design solid-state reactions targeting metastable materials. Here, we introduce a theoretical framework to predict and control polymorph selectivity in solid-state reactions. This framework presents reaction energy as a rarely used handle for polymorph selection, which influences the role of surface energy in promoting the nucleation of metastable phases. Through in situ characterization and density functional theory calculations on two distinct synthesis pathways targeting LiTiOPO 4 , we demonstrate how precursor selection and its effect on reaction energy can effectively be used to control which polymorph is obtained from solid-state synthesis. A general approach is outlined to quantify the conditions under which metastable polymorphs are experimentally accessible. With comparison to historical data, this approach suggests that using appropriate precursors could enable targeted materials synthesis across diverse chemistries through selective polymorph nucleation.

36 MATERIALS SCIENCE↗

Thermal-history dependent magnetoelastic transition in (Mn,Fe){sub 2}(P,Si)

The thermal-history dependence of the magnetoelastic transition in (Mn,Fe){sub 2}(P,Si) compounds has been investigated using high-resolution neutron diffraction. As-prepared samples display a large difference in paramagnetic-ferromagnetic (PM-FM) transition temperature compared to cycled samples. The initial metastable state transforms into a lower-energy stable state when the as-prepared sample crosses the PM-FM transition for the first time. This additional transformation is irreversible around the transition temperature and increases the energy barrier which needs to be overcome through the PM-FM transition. Consequently, the transition temperature on first cooling is found to be lower than on subsequent cycles characterizing the so-called “virgin effect.” High-temperature annealing can restore the cycled sample to the high-temperature metastable state, which leads to the recovery of the virgin effect. A model is proposed to interpret the formation and recovery of the virgin effect.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

THE SHOENBERG EFFECT IN A RELATIVISTIC DEGENERATE ELECTRON GAS AND OBSERVATIONAL EVIDENCE IN MAGNETARS

The electron gas inside a neutron star is highly degenerate and relativistic. Due to electron-electron magnetic interactions, the differential susceptibility can equal or exceed one, which causes the magnetic system of the neutron star to become metastable or unstable. The Fermi liquid of nucleons under the crust can be in a metastable state, while the crust is unstable to the formation of layers of alternating magnetization. The change of the magnetic stress acting on adjacent domains can result in a series of shifts or fractures in the crust. The release of magnetic free energy and elastic energy in the crust can cause the bursts observed in magnetars. Simultaneously, a series of shifts or fractures in the deep crust that is close to the Fermi liquid of nucleons can trigger a phase transition of the Fermi liquid of nucleons from a metastable state to a stable state. The magnetic free energy released in the Fermi liquid of nucleons corresponds to the giant flares observed in some magnetars.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Hidden disorder in the [alpha];#8242;;#8594;[sigma] transformation of Pu-1.9 at. % Ga

Enthalpy and entropy are thermodynamic quantities critical to determining how and at what temperature a phase transition occurs. At a phase transition, the enthalpy and temperature-weighted entropy differences between two phases are equal ({Delta}H=T{Delta}S), but there are materials where this balance has not been experimentally or theoretically realized, leading to the idea of hidden order and disorder. In a Pu-1.9 at. % Ga alloy, the {delta} phase is retained as a metastable state at room temperature, but at low temperatures, the {delta} phase yields to a mixed-phase microstructure of {delta}- and {alpha}{prime}-Pu. The previously measured sources of entropy associated with the {alpha}{prime} {yields} {delta} transformation fail to sum to the entropy predicted theoretically. We report an experimental measurement of the entropy of the {alpha}{prime} {yields} {delta} transformation that corroborates the theoretical prediction, and implies that only about 65% of the entropy stabilizing the {delta} phase is accounted for, leaving a missing entropy of about 0.5 k{sub B}/atom. Some previously proposed mechanisms for generating entropy are discussed, but none seem capable of providing the necessary disorder to stabilize the {delta} phase. This hidden disorder represents multiple accessible states per atom within the {delta} phase of Pu that may not be included in our current understanding of the properties and phase stability of {delta}-Pu.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Reading data stored in the state of metastable defects in silicon using band-band photoluminescence: Proof of concept and physical limits to the data storage density

The state of bistable defects in crystalline silicon such as iron-boron pairs or the boron-oxygen defect can be changed at room temperature. In this letter, we experimentally demonstrate that the chemical state of a group of defects can be changed to represent a bit of information. The state can then be read without direct contact via the intensity of the emitted band-band photoluminescence signal of the group of defects, via their impact on the carrier lifetime. The theoretical limit of the information density is then computed. The information density is shown to be low for two-dimensional storage but significant for three-dimensional data storage. Finally, we compute the maximum storage capacity as a function of the lower limit of the photoluminescence detector sensitivity.

36 MATERIALS SCIENCE↗

Overview: Understanding nucleation phenomena from simulations of lattice gas models

Monte Carlo simulations of homogeneous and heterogeneous nucleation in Ising/lattice gas models are reviewed with an emphasis on the general insight gained on the mechanisms by which metastable states decay. Attention is paid to the proper distinction of particles that belong to a cluster (droplet), that may trigger a nucleation event, from particles in its environment, a problem crucial near the critical point. Well below the critical point, the lattice structure causes an anisotropy of the interface tension, and hence nonspherical droplet shapes result, making the treatment nontrivial even within the conventional classical theory of homogeneous nucleation. For temperatures below the roughening transition temperature facetted crystals rather than spherical droplets result. The possibility to find nucleation barriers from a thermodynamic analysis avoiding a cluster identification on the particle level is discussed, as well as the question of curvature corrections to the interfacial tension. For the interpretation of heterogeneous nucleation at planar walls, knowledge of contact angles and line tensions is desirable, and methods to extract these quantities from simulations will be mentioned. Finally, also the problem of nucleation near the stability limit of metastable states and the significance of the spinodal curve will be discussed, in the light of simulations of Ising models with medium range interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A portable optical emission spectroscopy-cavity ringdown spectroscopy dual-mode plasma spectrometer for measurements of environmentally important trace heavy metals: Initial test with elemental Hg

A portable optical emission spectroscopy-cavity ringdown spectroscopy (OES-CRDS) dual-mode plasma spectrometer is described. A compact, low-power, atmospheric argon microwave plasma torch (MPT) is utilized as the emission source when the spectrometer is operating in the OES mode. The same MPT serves as the atomization source for ringdown measurements in the CRDS mode. Initial demonstration of the instrument is carried out by observing OES of multiple elements including mercury (Hg) in the OES mode and by measuring absolute concentrations of Hg in the metastable state 6s6p {sup 3}P{sub 0} in the CRDS mode, in which a palm-size diode laser operating at a single wavelength 405 nm is incorporated in the spectrometer as the light source. In the OES mode, the detection limit for Hg is determined to be 44 parts per 10{sup 9} (ppb). A strong radiation trapping effect on emission measurements of Hg at 254 nm is observed when the Hg solution concentration is higher than 50 parts per 10{sup 6} (ppm). The radiation trapping effect suggests that two different transition lines of Hg at 253.65 nm and 365.01 nm be selected for emission measurements in lower (<50 ppm) and higher concentration ranges (>50 ppm), respectively. In the CRDS mode, the detection limit of Hg in the metastable state 6s6p {sup 3}P{sub 0} is achieved to be 2.24 parts per 10{sup 12} (ppt) when the plasma is operating at 150 W with sample gas flow rate of 480 mL min{sup -1}; the detection limit corresponds to 50 ppm in Hg sample solution. Advantage of this novel spectrometer has two-fold, it has a large measurement dynamic range, from a few ppt to hundreds ppm and the CRDS mode can serve as calibration for the OES mode as well as high sensitivity measurements. Measurements of seven other elements, As, Cd, Mn, Ni, P, Pb, and Sr, using the OES mode are also carried out with detection limits of 1100, 33, 30, 144, 576, 94, and 2 ppb, respectively. Matrix effect in the presence of other elements on Hg measurements has been found to increase the detection limit to 131 ppb. These elements in lower concentrations can also be measured in the CRDS mode when a compact laser source is available to be integrated into the spectrometer in the future. This exploratory study demonstrates a new instrument platform using an OES-CRDS dual-mode technique for potential field applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Pathways for oxygen-isotope exchange in two model oxide clusters

Studies of oxygen-isotope-exchanges in two classes of polyoxoions have uncovered some similarities in reaction steps that are also consistent with mineral-dissolution studies. Here, the molecules were polyoxocations of Group 13 and polyoxoanions of Group 5, and the work was motivated by a desire to understand the dissolution of oxide minerals at the molecular scale. Experimentally, oxygen-isotope-exchange rates are found to be intensely sensitive to single-atom substitutions in the structures, even at sites that are otherwise inert. Exchange rates for different structural oxygen sites span several orders of magnitude, yet most oxygens within a molecule exhibit similar pH dependencies to isotopic exchange and these seem to reflect an average proton affinity of the ion. Single-atom substitutions have a dramatic affect on both the pH dependences of oxygen-isotope-exchanges and the overall reactivity of oxygen sites. Molecular dynamic and electronic-structure calculations identify similar steps in the pathways for exchange – (i) solvation forces cause a near-surface metal to detach from an underlying overbonded oxygen. (ii) This newly undercoordinated metal adds an isotopically normal oxygen as either a water, a hydronium ion or an hydroxide ion. (iii) Protons transfer from these adducts to more basic oxygens in the metastable structure. (iv) The metastability is longlived but access to the metastable state depends on the composition and symmetry of the starting structure, which is why single-atom substitutions are so important. (v) Within the metastable structure, oxygens shuffle positions and the metastable state collapses back into a more stable form. Pathways to form these metastable structures depend on the symmetry and composition of the starting geometry, which probably can't be adequately constrained for meaningful simulation at mineral surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hot-carrier dynamics in InAs/AlAsSb multiple-quantum wells

A type-II InAs/AlAs 0.16 Sb 0.84 multiple-quantum well sample is investigated for the photoexcited carrier dynamics as a function of excitation photon energy and lattice temperature. Time-resolved measurements are performed using a near-infrared pump pulse, with photon energies near to and above the band gap, probed with a terahertz probe pulse. The transient terahertz absorption is characterized by a multi-rise, multi-decay function that captures long-lived decay times and a metastable state for an excess-photon energy of >100 meV. For sufficient excess-photon energy, excitation of the metastable state is followed by a transition to the long-lived states. Excitation dependence of the long-lived states map onto a nearly-direct band gap (E g ) density of states with an Urbach tail below E g . As temperature increases, the long-lived decay times increase < E g , due to the increased phonon interaction of the unintentional defect states, and by phonon stabilization of the hot carriers > E g . Additionally, Auger (and/or trap-assisted Auger) scattering above the onset of the plateau may also contribute to longer hot-carrier lifetimes. Meanwhile, the initial decay component shows strong dependence on excitation energy and temperature, reflecting the complicated initial transfer of energy between valence-band and defect states, indicating methods to further prolong hot carriers for technological applications.

14 SOLAR ENERGY↗

Experimental Investigation of Organic Synthesis in Hydrothermal Environments

Seafloor hydrothermal systems may be the most likely locations on the early Earth for the emergence of life. Because of the disequilibrium inherent in such dynamic, mixing environments, abundant chemical energy would have been available for formation of the building blocks of life. In addition, theoretical studies suggest that organic compounds in these conditions would reach metastable states, due to kinetic barriers to the formation of stable equilibrium products (CO2 and methane). The speciation of organic carbon in metastable states is highly dependent on the oxidation state, pH, temperature, pressure and bulk composition of the system. The goal of our research is to investigate the effects of a number external variables on the formation, transformation, and stability of organic compounds at hydrothermal conditions. We have begun experimental work to attempt to control the oxidation state of simulated hydrothermal systems by using buffers composed of mineral powders and gas mixtures. We are also beginning to test the stability of organic compounds under these conditions. The experiments are being performed using the hydrothermal bomb apparatus at the U.S. Geological Survey in Menlo Park, CA and the supercritical water oxidizer (SCWO) at NASA Ames Research Center in Moffet Field, CA. The amino acids decomposed rapidly. Even after the approximately 15 minutes between addition of the amino acids and the first sampling, no amino acids were detected in the PPM system by GC- MS, while in the FeFeO system the amino acids were present at a level of less than 50% of original. Carboxylic acids, ammonia, and CO2 were the main products, along with some unidentified compounds. The ratios of carboxylic acids and concentrations of other products seem to have remained stable during the experiments, consistent with observations of other metastable systems and theoretical predictions.

Shock, Everett L.↗

Shape Effect in Layering of Solid Solutions in Small Volume: Bismuth–Antimony Alloy

The regularities of the effect of the shape of interphase boundaries in small volume systems on the separation of solutions with an upper critical solution temperature (UCST) are described by the example of Bi–Sb alloy particles with a core–shell configuration. The change in the shape of interphase boundaries is simulated in general by introducing a parameter corresponding to the degree of deviation of the shape of the boundaries from the spherical one. An analysis of the extrema of the Gibbs function revealed regularities in the effect of the shape of the core and shell phases on phase equilibria, the thermodynamic stability of heterogeneous states, and the phase separation diagram. The deviation of the shape of the interphase boundaries from the spherical shape changes the UCST and the mutual solubility of the components. The deformation of the shell of a core–shell particle increases the thermodynamic stability of the heterogeneous state, which contributes to the separation of the solution. The deformation of the core lowers the thermodynamic stability of the heterogeneous state and expands the range of metastable states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Experimental Investigation of Organic Synthesis in Hydrothermal Environments

The results of the investigation were presented at a Astrobiology Institute General Meeting. Seafloor hydrothermal systems may be the most likely locations on the early Earth for the emergence of life. Because of the disequilibrium inherent in such dynamic, mixing environments, abundant chemical energy would have been available for formation of the building blocks of life. In addition, theoretical studies suggest that organic compounds in these conditions would reach metastable states, due to kinetic barriers to the formation of stable equilibrium products (CO2 and methane). The speciation of organic carbon in metastable states is highly dependent on the oxidation state, pH, temperature, pressure and bulk composition of the system. The goal of our research is to investigate the effects of a number external variables on the formation, transformation, and stability of organic compounds at hydrothermal conditions. We have begun experimental work to attempt to control the oxidation state of simulated hydrothermal systems by using buffers composed of mineral powders and gas mixtures. We are also beginning to test the stability of organic compounds under these conditions.

Shock, Everett L.↗

Correlation buildup during recrystallization in three-dimensional dusty plasma clusters

The recrystallization process of finite three-dimensional dust clouds after laser heating is studied experimentally. The time-dependent Coulomb coupling parameter is presented, showing that the recrystallization starts with an exponential cooling phase where cooling is slower than damping by the neutral gas friction. At later times, the coupling parameter oscillates into equilibrium. It is found that a large fraction of cluster states after recrystallization experiments is in metastable states. The temporal evolution of the correlation buildup shows that correlation occurs on even slower time scale than cooling.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

On the irreversible dynamics emerging from quantum resonances

We consider the dynamics of quantum systems which possess stationary states as well as slowly decaying, metastable states arising from the perturbation of bound states. We give a decomposition of the propagator into a sum of a stationary part, one exponentially decaying in time and a polynomially decaying remainder. The exponential decay rates and the directions of decay in Hilbert space are determined, respectively, by complex resonance energies and by projections onto resonance states. Our approach is based on an elementary application of the Feshbach map. It is applicable to open quantum systems and to situations where spectral deformation theory fails. We derive a detailed description of the dynamics of the spin-boson model at arbitrary coupling strength.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Argon plasma modeling with detailed fine-structure cross sections

Our recently reported fully relativistic distorted-wave electron-impact cross sections from the ground and metastable states of argon to various excited fine-structure levels are incorporated in a collisional-radiative model to obtain the population densities for the 3p{sup 5}4s and 3p{sup 5}4p (1s and 2p) fine-structure manifolds for low temperature argon plasmas. Excitation cross sections from the two 3p{sup 5}4s J = 1 resonance levels, 1s{sub 2} and 1s{sub 4}, to the higher lying 2p fine-structure manifold as well as for transitions among individual levels of the 1s and 2p manifolds are also calculated and included in the present model which were not fully considered in any earlier model. Our results for the population densities of the 1s and 2p levels show good agreement with recent measurements. The variation of population densities of all the 1s and 2p levels with electron temperature and density are presented. We have also calculated and compared the intensities for the 750.38 nm (2p{sub 1}{yields} 1s{sub 2}) and 696.54 nm (2p{sub 2}{yields} 1s{sub 5}) lines with recently reported experimental results. The present work suggests that the inclusion of a complete fine-structure description of the electronic processes occurring in the plasma is important for a collisional radiative model, which includes separate 1s and 2p levels.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Persistent opto-ferroelectric responses in molecular ferroelectrics

Persistent photoresponses require optical excitations to metastable states, which are rare of ionic origin due to the indirect photon-ion interaction. In this work, we explore the photoinduced metastable proton states in the proton-transfer type molecular ferroelectric croconic acid.We observe that, after the photoexcitation, the changes of structural and ferroelectric properties relax in ~10 3 s, indicating persistent photoresponses of ionic origin. In contrast, the photoconductivity relaxes within 1 s. The 10 3 s timescale suggests that the ionic metastable states result from proton transfer both along and out of the hydrogen bonds. Furthermore, this discovery unveils an ionic mechanism for the phototunability, which offers persistent opto-ferroelectric control for proton-transfer type molecular ferroelectrics.

36 MATERIALS SCIENCE↗