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At least 1,297 records · Page 72

Solvent-Induced Shift of Spectral Lines in Polar–Polarizable Solvents

Solvent-induced shift of optical transition lines is traditionally described by the Lippert- McRae equation given in terms of the Onsager theory for dipole solvation. It splits the overall shift into the equilibrium solvation by induced dipoles and the reaction field by the permanent dipoles in equilibrium with the chromophore in the ground state. Here we have reconsidered this classical problem from the perspective of microscopic solvation theories. A microscopic solvation functional is derived and continuum solvation is consistently introduced by taking the limit of zero wavevector in the reciprocal-space solvation susceptibility functions. We show that the phenomenological expression for the reaction field of permanent dipoles in the Lippert-McRae equation is not consistent with the microscopic theory. The main deficiency of the Lippert- McRae equation equation is the use of additivity of the response by permanent and induced dipoles of the liquid. An alternative closed-form equation for the spectral shift is derived. Its continuum limit allows a new, non-additive functionality for the solvent-induced shift in terms of the high-frequency and static dielectric constants. Finally, the main qualitative outcome of the theory is a significantly weaker dependence of the spectral shift on the polarizability of the solvent than predicted by the Lippert-McRae formula.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electronic Interactions of Size-Selected Oxide Clusters on Metallic and Thin Film Oxide Supports

The interfacial electronic structure of various size-selected metal oxide nanoclusters (M 3 O x ; M = Mo, Nb, Ti) on Cu(111) and a thin film of Cu 2 O supports were investigated in this paper by a combination of experimental methods and density functional theory (DFT). These systems explore electron transfer at the metal–metal oxide interface which can modify surface structure, metal oxidation states, and catalytic activity. Electron transfer was probed by measurements of surface dipoles derived from coverage dependent work function measurements using two-photon photoemission (2PPE) and metal core level binding energy spectra from X-ray photoelectron spectroscopy (XPS). The measured surface dipoles are negative for all clusters on Cu(111) and Cu 2 O/Cu(111), but those on the Cu 2 O surface are much larger in magnitude. In addition, sub-stoichiometric or “reduced” clusters exhibit smaller surface dipoles on both the Cu(111) and Cu 2 O surfaces. Negative surface dipoles for clusters on Cu(111) suggest Cu → cluster electron transfer, which is generally supported by DFT-calculated Bader charge distributions. For Cu 2 O/Cu(111), calculations of the surface electrostatic potentials show that the charge distributions associated with cluster adsorption structures or distortions at the cluster–Cu 2 O–Cu(111) interface are largely responsible for the observed negative surface dipoles. Changes observed in the XPS spectra for the Mo 3d, Nb 3d, and Ti 2p core levels of the clusters on Cu(111) and Cu 2 O/Cu(111) are interpreted with help from the calculated Bader charges and cluster adsorption structures, the latter providing information about the presence of inequivalent cation sites. Finally, the results presented in this work illustrate how the combined use of different experimental probes along with theoretical calculations can result in a more realistic picture of cluster–support interactions and bonding.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Non-resonant Raman optical activity from phase-space electronic structure theory

In order to model experimental non-resonant Raman optical activity, chemists must compute a host of second-order response tensors (e.g., the electric-dipole–magnetic-dipole polarizability) and their nuclear derivatives along a set of vibrational modes. While these response functions are almost always computed within a Born–Oppenheimer (BO) framework, here we provide a natural interpretation of the electric-dipole–magnetic-dipole polarizability within phase space electronic structure theory, a beyond-BO model whereby the electronic structure depends on nuclear momentum (P) in addition to nuclear position (R). By coupling to nuclear momentum, phase space electronic structure theory is able to capture the asymmetric response of the electronic properties to an external field, in so far as for a vibrating (non-stationary) molecule, $\frac{∂μ}{∂B}$≠$\frac{∂m}{∂F}$, where μ and m are the electrical linear and magnetic dipoles, and F and B are electric and magnetic fields. As an example, for a prototypical methyloxirane molecule, we show that phase space electronic structure theory is able to deliver a reasonably good match with experimental results in a manner that is formally invariant to gauge origin G 0 —provided that one uses a complete basis or, alternatively, gauge invariant atomic orbitals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exploring charge transport dynamics in a cryogenic P-type germanium detector

Abstract This study explores the dynamics of charge transport within a cryogenic P-type Ge particle detector, fabricated from a crystal cultivated at the University of South Dakota. By subjecting the detector to cryogenic temperatures and an Am-241 source, we observe evolving charge dynamics and the emergence of cluster dipole states, leading to the impact ionization process at 40 mK. Our analysis focuses on crucial parameters: the zero-field cross-section of cluster dipole states and the binding energy of these states. For the Ge detector in our investigation, the zero-field cross-section of cluster dipole states is determined to be 8.45 × 10 −11 ± 4.22 × 10 −12 cm 2 . Examination of the binding energy associated with cluster dipole states, formed by charge trapping onto dipole states during the freeze-out process, reveals a value of 0.034 ± 0.0017 meV. These findings shed light on the intricate charge states influenced by the interplay of temperature and electric field, with potential implications for the sensitivity in detecting low-mass dark matter.

Physics↗

Generation of out-of-plane ferroelectric behavior in a one-atom-thick monolayer

Ferroelectricity with out-of-plane polarization has so far been found in several two-dimensional (2D) materials, including monolayers comprising three to five planes of atoms, e.g. α-In 2 Se 3 and MoTe 2 . Here, we explore the generation of out-of-plane polarization within a one-atom-thick monolayer material, namely hexagonal boron nitride. We performed density-functional-theory calculations to explore inducing ferroelectric-like distortions through incorporation of isovalent substitutional impurities that are larger than the host atoms. This disparity in bond lengths causes a buckling of the h-BN, either up or down, which amounts to a dipole with two equivalent energies and opposing orientations. We tested several impurities to explore the magnitude of the induced dipole and the switching energy barrier for dipole inversion. The effects of strain, dipole–dipole interactions, and vertical heterostructures with graphene are further explored. Our results suggest a highly-tunable system with ground state antiferroelectricity and metastable ferroelectricity. Finally, we expect that this work will help foster new ways to include functionality in layered 2D-material-based applications.

36 MATERIALS SCIENCE↗

Dipolar quantum logic for freely rotating trapped molecular ions

We consider the practical feasibility of using the direct, electric dipole-dipole interaction between cotrapped molecular ions for robust quantum logic without the need for static polarizing fields. Here, the use of oscillating dipole moments, as opposed to static electric dipoles, dynamically decouples the dipoles from laboratory fields, including the electric fields of the trap itself. Further, this implementation does not require the quantum control of motion, potentially removing a major roadblock to ion trap quantum computing scalability. Since the polarizing field is electromagnetic radiation, even pairs of states with splittings in the THz regime can be fully polarized.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Experimental M 1 response of 40 Ar as a benchmark for neutrino-nucleus scattering calculations

The excitation of atomic nuclei via magnetic dipole transitions is closely related to the inelastic neutral-current neutrino-nucleus (NC-νA) scattering process due to the similarity of the transition operators. NC-νA-scattering serves for the detection of supernova neutrinos and poses a significant source of background in modern liquid-argon based high-energy neutrino detection experiments. To enable tests of the reliability of predictions for neutrino-nucleus scattering, the magnetic dipole response of 40 Ar below 7.7 MeV was characterized in a nuclear resonance fluorescence experiment using quasimonoenergetic γ-ray beams. The linear polarization of the beams allowed for assignments of electric or magnetic character to previously known dipole excitations. A total magnetic dipole strength of $0.36$ $^{+0.04}_{–0.05}$ $μ$ $^{2}_{N}$ was identified in the energy range of the present experiment. Combined with data from previous measurements, the full magnetic dipole strength of 40 Ar below the neutron separation threshold was investigated. Due to the low background in the energy range within the bandwidth of the γ-ray beams, the previous sensitivity limit was improved. Furthermore, a large-scale nuclear shell model calculation in the sd–fp space satisfactorily agrees with the data in terms of excitation energies and strengths of the observed 1 + states.

39 ≤ A ≤ 58↗

Impulsive Magnetic Anomaly Detection At the 100-m Scale With an Array of Induction Coil Magnetometers

We demonstrate magnetic anomaly detection (MAD) using an array of 24 commercial induction coil magnetometers with stand-off distances from a pulsed 99.8(3) kA·m 2 magnetic dipole source of 260–1200 m. The sparse array is used to estimate the magnetic dipole location, magnitude, and orientation. We demonstrate how independent component analysis (ICA) improves the accuracy and precision of the magnetometer array when estimating the dipole parameters. Using sensor responses recorded from individual source pulses, we estimate the dipole location to within 29 ± 2 m, the magnitude to within 3 ± 3 kA·m 2 , and dipole orientation error to within 19 ± 0.6°.

47 OTHER INSTRUMENTATION↗

A Nonlinear Theory of Atmospheric Blocking: A Potential Vorticity Gradient View

In this paper, an extended nonlinear multiscale interaction model of blocking events in the equivalent barotropic atmosphere is used to investigate the effect of a slowly varying zonal wind in the meridional direction on dipole blocking that is regarded as a nonlinear Rossby wave packet. It is shown that the meridional gradient of potential vorticity [Formula: see text] prior to the blocking onset, which is related to the background zonal wind and its nonuniform meridional shear, can significantly affect the lifetime, intensity, and north–south asymmetry of dipole blocking, while the blocking dipole itself is driven by preexisting incident synoptic-scale eddies. The magnitude of the background PV y determines the energy dispersion and nonlinearity of blocking. It is revealed that a small background PV y is a prerequisite for strong and long-lived eddy-driven blocking that behaves as a persistent meandering westerly jet stream, while the blocking establishment further reduces the PV y within the blocking region, resulting in a positive feedback between blocking and PV y . When the core of the background westerly jet shifts from higher to lower latitudes, the blocking shows a northwest–southeast-oriented dipole with a strong anticyclonic anomaly to the northwest and a weak cyclonic anomaly to the southeast as its northern pole moves westward more rapidly and has weaker energy dispersion and stronger nonlinearity than its southern pole because of the smaller PV y in higher latitudes. The opposite is true when the background jet shifts toward higher latitudes. The asymmetry of dipole blocking vanishes when the background jet shows a symmetric double-peak structure. Thus, a small prior PV y is a favorable precursor for the occurrence of long-lived and large-amplitude blocking.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tailoring dielectric resonator geometries for directional scattering and Huygens’ metasurfaces

In this paper we describe a methodology for tailoring the design of metamaterial dielectric resonators, which represent a promising path toward low-loss metamaterials at optical frequencies. We first describe a procedure to decompose the far field scattered by subwavelength resonators in terms of multipolar field components, providing explicit expressions for the multipolar far fields. We apply this formulation to confirm that an isolated high-permittivity dielectric cube resonator possesses frequency separated electric and magnetic dipole resonances, as well as a magnetic quadrupole resonance in close proximity to the electric dipole resonance. We then introduce multiple dielectric gaps to the resonator geometry in a manner suggested by perturbation theory, and demonstrate the ability to overlap the electric and magnetic dipole resonances, thereby enabling directional scattering by satisfying the first Kerker condition. We further demonstrate the ability to push the quadrupole resonance away from the degenerate dipole resonances to achieve local behavior. These properties are confirmed through the multipolar expansion and show that the use of geometries suggested by perturbation theory is a viable route to achieve purely dipole resonances for metamaterial applications such as wave-front manipulation with Huygens’ metasurfaces. Our results are fully scalable across any frequency bands where high-permittivity dielectric materials are available, including microwave, THz, and infrared frequencies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

From Feast to Famine: A Systematic Study of Accretion onto Oblique Pulsars with 3D GRMHD Simulations

Disk-fed accretion onto neutron stars can power a wide range of astrophysical sources ranging from X-ray binaries, to accretion-powered millisecond pulsars, ultraluminous X-ray sources, and gamma-ray bursts. A crucial parameter controlling the gas–magnetosphere interaction is the strength of the stellar dipole. In addition, coherent X-ray pulsations in many neutron star systems indicate that the star's dipole moment is oblique relative to its rotation axis. Therefore, it is critical to systematically explore the 2D parameter space of the star's magnetic field strength and obliquity, which is what this work does, for the first time, in the framework of 3D general-relativistic magnetohydrodynamics. If the accretion disk carries its own vertical magnetic field, this introduces an additional factor: the relative polarity of the disk and stellar magnetic fields. We find that depending on the strength of the stellar dipole and the star–disk relative polarity, the neutron star's jet power can either increase or decrease with increasing obliquity. For weak dipole strength (equivalently, high accretion rate), the parallel polarity results in a positive correlation between jet power and obliquity, whereas the antiparallel orientation displays the opposite trend. For stronger dipoles, the relative-polarity effect disappears, and jet power always decreases with increasing obliquity. The influence of the relative polarity gradually disappears as obliquity increases. Highly oblique pulsars tend to have an increased magnetospheric radius, a lower mass accretion rate, and enter the propeller regime at lower magnetic moments than aligned stars.

79 ASTRONOMY AND ASTROPHYSICS↗

Equivalent source modeling of the main field using Magsat data

A graphic software package was developed to plot the dipole positions for a particular model on a world map. An arrow is drawn at each dipole in the direction of the horizontal magnetization vector, with length proportional to the horizontal magnitude. A contouring package represents the radical component of the magnetization vector. Based on quiet Magsat data, several dipole models were derived. These are being verified against each other and against MGST (6/80) data set as to goodness of fit and stability of solution. The spatial power spectra computed from spherical harmonic expansions of the dipole models is being analyzed relative to crustal and core content. The power spectra for one of the dipole models and a spherical harmonic model based on Magsat data through degree and order 23 is presented.

Source record↗

Theoretical calculation of ozone vibrational infrared intensities

An ab initio dipole moment function for ozone has been computed using the CASSCF (complete active space self-consistent field) method, and forms the basis for a calculation of ozone infrared band intensities. Vibrational wave functions were generated using the variational method with potential energy surfaces derived from experimental force constants. Computed values of the permanent dipole moment, dipole moment derivatives, and infrared band strengths are all found to be in remarkably good agreement with experiment. Intensities are predicted for hot bands for which experimental values are unavailable, and implications for atmospheric ozone spectroscopy are discussed. As the dipole moment matrix element signs are now established for nearly all of the observed bands, further refinement of the dipole moment function is possible.

Adler-Golden, S. M.↗

Measurements of Siple transmitter signals on the DE 1 satellite - Wave normal direction and antenna effective length

A new experimental technique is developed to simultaneously measure the wave propagation direction and the effective length of a small (L value much smaller than wavelength) electric dipole antenna on a spin-stabilized satellite in the magnetosphere. The technique relies on the near simultaneous measurement of single components of the electric and magnetic fields of a coherent VLF signal injected into the medium from a ground-based source. The spin fading characteristics of the signal received by the electric dipole and the magnetic loop antenna permit the measurement of the wave normal direction assuming whistler-mode propagation. In-situ and remote measurements of the local cold plasma density are used to determine the refractive index. The wave electric field is then inferred from the wave magnetic field as measured on the loop antenna, the refractive index and the direction of propagation. Comparing this electric field with the measured voltage across the dipole antenna leads to the determination of the effective length of the receiving electric dipole. The technique is applied to data from the Dynamics Explorer 1 satellite observations of whistler mode signals injected into the magnetosphere from the Siple, Antarctica, VLF transmitter. In one case, with the measured background cold plasma density being 15 el/cu cm, the effective length of the 200 m-long electric dipole antenna is found to be 222 + or - 56 m, i.e., about twice the conventional value.

Sonwalker, V. S.↗

The source surface and photospheric magnetic field models

It is possible to reproduce the configuration of the neutral line on the solar source surface by the axial dipole at the center of the sun and a few fictitious dipoles on the photosphere. An attempt is made to identify the nature of such fictitious dipoles in the photospheric magnetic fields. It is shown that large-scale photospheric dipole fields can be identified clearly at the locations indicated by the fictitious dipoles when the photospheric field is very simple. They are found to be active regions.

Saito, T.↗

Venus internal magnetic field and its interaction with the interplanetary magnetic field

In a previous study, Knudsen et al. suggested that Venus has a weak internal magnetic dipole field of the order of 7 x 10 + 20 G cm(exp -3) that is manifested in the form of magnetic flux tubes threading the ionospheric holes in the Venus nightside ionosphere. They pointed out that any internal field of Venus, dipole or multipole, would be weakened in the subsolar region and concentrated in the antisolar region of the planet by the supersonic transterminator convection of the dayside ionosphere into the nightside hemisphere. The inferred magnitude of the dipole field does not violate the upper limit for an internal magnetic field established by the Pioneer Venus magnetometer experiment. The most compelling objection to the model suggested by Knudsen et al. has been the fact that it does not explain the observed interplanetary magnetic field (IMF) control of the polarity of the ionospheric hole flux tubes. In this presentation I suggest that a magnetic reconnection process analogous to that occurring at earth is occurring at Venus between the IMF and a weak internal dipole field. At Venus in the subsolar region, the reconnection occurs within the ionosphere. At Earth it occurs at the magnetopause. Reconnection will occur only when the IMF has an appropriate orientation relative to that of the weak internal field. Thus, reconnection provides a process for the IMF to control the flux tube polarity. The reconnection in the subsolar region takes place in the ionosphere as the barrier magnetic field is transported downward into the lower ionosphere by downward convection of ionospheric plasma and approaches the oppositely directed internal magnetic field that is diffusing upward. The reconnected flux tubes are then transported anti-Sunward by the anti-Sunward convecting ionospheric plasma as well as by the anti-Sunward-flowing solar wind. Reconnection will also occur in the Venus magnetic tail region, somewhat analogously to the reconnection that occurs in the magnetotail of the Earth. The possibility that reconnection is occurring between the IMF and an internal dipole field may be tested by measuring the orientation of the IMF projected into a plane perpendicular to the solar wind velocity during time intervals for which ionospheric holes are observed. The orientations of the IMV components should fall within a 180 deg angle.

Knudsen, W. C.↗

BATSE Observations of the Large-Scale Isotropy of Gamma-Ray Bursts

We use dipole and quadrupole statistics to test the large-scale isotropy of the first 1005 gamma-ray bursts observed by the Burst and Transient Source Experiment (BATSE). In addition to the entire sample of 1005 gamma-ray bursts, many subsets are examined. We use a variety of dipole and quadrupole statistics to search for Galactic and other predicted anisotropies and for anisotropies in a coordinate-system independent manner. We find the gamma-ray burst locations to be consistent with isotropy, e.g., for the total sample the observed Galactic dipole moment (cos theta) differs from the value predicted for isotropy by 0.9 sigma and the observed Galactic quadrupole moment (sin(exp 2) b - 1/3) by 0.3 sigma. We estimate for various models the anisotropies that could have been detected. If one-half of the locations were within 86 deg of the Galactic center, or within 28 deg of the Galactic plane, the ensuing dipole or quadrupole moment would have typically been detected at the 99% confidence level. We compare the observations with the dipole and quadrupole moments of various Galactic models. Several Galactic gamma-ray bursts models have moments within 2 sigma of the observations; most of the Galactic models proposed to date are no longer in acceptable agreement with the data. Although a spherical dark matter halo distribution could be consistent with the data, the required core radius is larger than the core radius of the dark matter halo used to explain the Galaxy's rotation curve. Gamma-ray bursts are much more isotropic than any observed Galactic population, strongly favoring but not requiring an origin at cosmological distances.

Briggs, Michael S.↗

"Electrostructural Phase Changes" In Charged Particulate Clouds: Planetary and Astrophysical Implications

There is empirical evidence that freely-suspended triboelectrostatically charged particulate clouds of dielectric materials undergo rapid conversion from (nominally) monodispersed "aerosols" to a system of well-defined grain aggregates after grain motion or fluid turbulence ceases within the cloud. In United States Microgravity Laboratory Space Shuttle experiments USML-1 and USML-2, it was found that ballistically-energized grain dispersions would rapidly convert into populations of filamentary aggregates after natural fluid (air) damping of grain motion. Unless continuously disrupted mechanically, it was impossible to maintain a non-aggregated state for the grain clouds of sand-size materials. Similarly, ground- based experiments with very fine dust-size material produced the same results: rapid, impulsive "collapse" of the dispersed grains into well-defined filamentary structures. In both ground-based and microgravity experiments, the chains or filaments were created by long-range dipole electrostatic forces and dipole-induced dielectric interactions, not by monopole interactions. Maintenance of the structures was assisted by short-range static boundary adhesion forces and van der Waals interactions. When the aggregate containers in the USML experiments were disturbed after aggregate formation, the quiescently disposed filaments would rearrange themselves into fractal bundles and tighter clusters as a result of enforced encounters with one another. The long-range dipole interactions that bring the grains together into aggregates are a product of randomly-distributed monopole charges on the grain surfaces. In computer simulations, it has been shown that when the force vectors of all the random charges (of both sign) on a grain are resolved mathematically by assuming Coulombic interaction between them, the net result is a dipole moment on individual grains, even though the grains are electrically neutral insofar as there is no predominance, on their surface, of one charge sign over another. The random charges of both sign derive from natural grain-to-grain interactions that produce triboelectrification via charge exchange every time grain surfaces make contact with one another. The conversion from a random distribution of grains (upon which there are randomly distributed charges) into an organization of electrostatically-ordered aggregates, can be regarded (within the framework of granular-material science) as an "electrical or Coulombic phase change" of the particulate cloud. It is not totally dissimilar from the more normal phase-change concept in which, for example, a gas with long free-path-molecules suddenly becomes a solid as a result of structural ordering of the molecules (notably, also the result of electronic forces, albeit at a different scale). In both the gas-to-solid case, and the aerosol-to-aggregate case, the same materials and charges are present before and after the phase change, but their arrangement now has a higher degree of order and a lower-energy configuration. An input of energy into the system is required to reverse the situation. The aggregates in the USML experiments were observed to undergo at least two phase changes as noted above. The point about phase changes, and by implication, the "electrostructural" reorganizations in particulate clouds, is the following: (a) they can occur very rapidly, almost spontaneously, above a critical cloud density, (b) in going from a higher energy state to a lower energy state, they convert to a denser system, (c) energy must be required to reverse the situation, implying that energy is released during the high-to-low energy phase change. In applying this information to natural particulate clouds, some inferences can be made (it is stressed that reference is still to dielectric materials attracted by dipole forces). There are several natural settings to which the USML observations apply, and to which the phase-change implications likewise apply. Dense clouds of triboelectrically-charged, kinetically-energized grains are to be found in volcanic eruptions (particularly on earth), aeolian dust storms (particularly on Mars), meteorite impact ejecta curtains (on all planets), in "immature" debris rings around planets (e.g., that from which our own Moon may have condensed), and in gravitationally collapsing protoplanetary dust/planetesimal debris disks where dielectric granules are being increasingly brought into collisional relationships with one another (increasing both charge exchange and physical proximity). It is noted that in many of these cases, the degree of electrical charging on the grains is likely to be much higher than that in the USML experiments where charging was not enhanced above the "normal", naturally encountered level for the particular materials (quartz, glass, and various silicate minerals). Application of the phase-change concept suggests that volcanic, aeolian, and impact debris clouds may, under certain circumstances, undergo rapid, impulsive, or even catastrophic collapse into a denser state that will lead to rapid precipitation or fall-out of suspended particulates. Although this idea has been suggested previously by the author , the phase change concept possibly permits some new insights into cloud-system behavior. For example, in a protoplanetary debris disk, the work of gravity may suddenly be enhanced by electrostatically driven collapse of the system when materials reach a critical intergranular spacing or grain number density. This might reduce the rate of planet formation by orders of magnitude (considering the ratio of g-forces to electrostatic ones for very small grains in close proximity), and indeed, it might drive the collapse into a system configuration that would perhaps not be created by gravity alone. Additional information is contained in the original.

Marshall, J. R.↗