Dipolar Contributions Research Articles

1s2p Resonant Inelastic X-ray Scattering Magnetic Circular Dichroism as a probe for the local and non-local orbitals in CrO2

We have determined the magnetic ground state of the half-metal CrO2 based on 1s2p Resonant Inelastic X-ray Scattering Magnetic Circular Dichroism (RIXS-MCD) experiments. The two-dimensional RIXS-MCD map displays the 1s X-ray absorption spectrum combined with the 1s2p X-ray emission decay, where there is a large MCD contrast in the final state involving the 2p core hole.Our measurements show that the Cr K pre-edge structure is dominated by dipolar contributions and the quadrupole peak is invisible in direct K pre-edge absorption. Using RIXS-MCD, we reveal that the quadrupole 1s3d pre-edge has a large MCD contrast, which appears at lower energy with respect to the K pre-edge maximum.We use crystal field multiplet calculations to model the excitonic RIXS-MCD spectral shape in tetragonal (D4h) symmetry. The RIXS-MCD is strongly sensitive to the ground state distortion of the Cr4+ sites. The calculations of the RIXS-MCD maps suggest that the 3d spin–orbit interaction is fully quenched (ζ3d=0meV) and the ground state electron configuration must contain a 3B2g (D4h) contribution, which is required to explain the appearance of the Magnetic Circular Dichroism (MCD) in the Cr K pre-edge. This is in apparent contrast with the compressed tetragonal distortion.

Electronic structure modification of theKTaO3single-crystal surface byAr+bombardment

Oxygen vacancies play an important role in controlling the physical properties of a perovskite oxide. We report alterations in the electronic properties of a cubic perovskite oxide, namely, ${\mathrm{KTaO}}_{3}$, as a function of oxygen vacancies. The conducting surface of the ${\mathrm{KTaO}}_{3}$ single-crystal substrate has been realized via ${\mathrm{Ar}}^{+}$ irradiation. The band gap changes as a function of conductivity which is controlled by irradiation time, indicating the formation of defect states. Kelvin probe force microscopy suggests a sharp increase in the work function upon ${\mathrm{Ar}}^{+}$ irradiation for a short period of time followed by a monotonic decrease, as we increase the irradiation time. Our experimental findings along with theoretical simulations suggest a significant surface dipole contribution and an unusual change in the electronic band line-up of ${\mathrm{KTaO}}_{3}$ due to oxygen vacancies.

On the projected mass distribution around galaxy clusters

Gravitational lensing allows to quantify the angular distribution of the convergence field around clusters of galaxies to constrain their connectivity to the cosmic web. We describe in this paper the corresponding theory in Lagrangian space where analytical results can be obtained by identifying clusters to peaks in the initial field. We derive the three-point Gaussian statistics of a two-dimensional field and its first and second derivatives. The formalism allows us to study the statistics of the field in a shell around a central peak, in particular its multipolar decomposition. The peak condition is shown to significantly remove power from the dipolar contribution and to modify the monopole and quadrupole. As expected, higher order multipoles are not significantly modified by the constraint. Analytical predictions are successfully checked against measurements in Gaussian random fields. The effect of substructures and radial weighting is shown to be small and does not change the qualitative picture. The non-linear evolution is shown to induce a non-linear bias of all multipoles proportional to the cluster mass.We predict the Gaussian and weakly non-Gaussian statistics of multipolar moments of a two-dimensional field around a peak as a proxy for the azimuthal distribution of the convergence field around a cluster of galaxies. A quantitative estimate of this multipolar decomposition of the convergence field around clusters in numerical simulations of structure formation and in observations will be presented in two forthcoming papers.

Near-infrared linewidth narrowing in plasmonic Fano-resonant metamaterials via tuning of multipole contributions

We report on an experimental and computational (multipole decomposition) study of Fano resonance modes in complementary near-IR plasmonic metamaterials. Resonance wavelengths and linewidths can be controlled by changing the symmetry of the unit cell so as to manipulate the balance among multipole contributions. In the present case, geometrically inverting one half of a four-slot (paired asymmetric double bar) unit cell design changes the relative magnitude of magnetic quadrupole and toroidal dipole contributions leading to the enhanced quality factor, figure of merit, and spectral tuning of the plasmonic Fano resonance.

Magnetic Dipole Scattering from Metallic Nanowire for Ultrasensitive Deflection Sensing.

It is generally believed that when a single metallic nanowire is sufficiently small, it scatters like a point electric dipole. We show theoretically when a metallic nanowire is placed inside specially designed beams, the magnetic dipole contribution along with the electric dipole resonance can lead to unidirectional scattering in the far field, fulfilling Kerker's condition. Remarkably, this far-field unidirectional scattering encodes information that is highly dependent on the nanowire's deflection at a scale much smaller than the wavelength. The special roles of small but essential magnetic response along with the plasmonic resonance are highlighted for this extreme sensitivity as compared with the dielectric counterpart. In addition, the same essential role of the magnetic dipole contribution is also presented for a very small metallic nanosphere.

Electric and Magnetic Dipole Strength at Low Energy.

A low-energy enhancement of radiative strength functions was deduced from recent experiments in several mass regions of nuclei, which is believed to impact considerably the calculated neutron capture rates. In this Letter we investigate the behavior of the low-energy γ-ray strength of the ^{44}Sc isotope, for the first time taking into account both electric and magnetic dipole contributions obtained coherently in the same theoretical approach. The calculations are performed using the large-scale shell-model framework in a full 1ℏω sd-pf-gds model space. Our results corroborate previous theoretical findings for the low-energy enhancement of the M1 strength but show quite different behavior for the E1 strength.

Physical conditions for Jupiter-like dynamo models

The Juno mission will measure Jupiter’s magnetic field with unprecedented precision and provide a wealth of additional data that will allow us to constrain the planet’s interior structure and dynamics. Here we analyse 66 different numerical simulations in order to explore the sensitivity of the dynamo-generated magnetic field to the planets interior properties. Jupiter field models based on pre-Juno data and up-to-date interior models based on ab initio simulations serve as benchmarks. Our results suggest that Jupiter-like magnetic fields can be found for a number of different models. These complement the steep density gradients in the outer part of the simulated shell with an electrical conductivity profile that mimics the low conductivity in the molecular hydrogen layer and thus renders the dynamo action in this region largely unimportant. We find that whether we assume an ideal gas or use the more realistic interior model based on ab initio simulations makes no difference. However, two other factors are important. A low Rayleigh number leads to a too strong axial dipole contribution while the axial dipole dominance is lost altogether when the convective driving is too strong. The required intermediate range that yields Jupiter-like magnetic fields depends on the other system properties. The second important factor is the convective magnetic Reynolds number radial profile Rmc(r), basically a product of the non-axisymmetric flow velocity and electrical conductivity. We find that the depth where Rmc exceeds about 50 is a good proxy for the top of the dynamo region. When the dynamo region sits too deep, the axial dipole is once more too dominant due to geometric reasons. Extrapolating our results to Jupiter and the result suggests that the Jovian dynamo extends to 95% of the planetary radius.The zonal flow system in our simulations is dominated by an equatorial jet which remains largely confined to the molecular layer. Where the jet reaches down to higher electrical conductivities, however, it gives rise to a secondary αΩ dynamo that modifies the dipole-dominated field produced deeper in the planet. This secondary dynamo can lead to strong magnetic field patches at lower latitudes that seem compatible with the pre-Juno field models.

Predicting the dielectric behavior of orange and other citrus fruit juices at 915 and 2450 MHz

ABSTRACTDielectric properties (DP: relative permittivity and loss factor) and electrical conductivity are important parameters for evaluating the microwave penetration depth and designing applicators for pasteurization processes. In this context, generalized equations that can predict the DP of a group of food products as a function of their characteristics are useful. The dielectric behaviours of eight citrus fruit juices (Pera, Lima, and Navel oranges, Ponkan tangerine, Murcott tangor, Mediterranean mandarin, Sicilian lemon, and Persian lime) and three Pera/Lima blends (25, 50, 75%) for temperatures between 0 and 90 °C and frequency between 500 and 3000 MHz were studied. The results were correlated with temperature at frequencies of 915 and 2450 MHz. It was possible to quantify the ionic and dipolar contributions. DPs were modelled based on the behaviour of pure water in a semiempirical approach using correction factors, which were correlated with temperature and juice physicochemical characteristics (pH, Brix, conductivity). Polynomial regressions can successfully predict relative permittivity with mean absolute errors of 0.49±0.35% and 0.58±0.48% and the loss factor with errors of 4.1±3.9% and 2.8±2.3% at 915 and 2450 MHz, respectively, for juices with Brix/acid ratio between 1.26 and 29.9.

Stability of Neel skyrmions in ultra-thin nanodots considering Dzyaloshinskii-Moriya and dipolar interactions

An analytical expression for the energy of Neel skyrmions in ultra-thin nanodots considering exchange, uniaxial anisotropy, Dzyaloshinskii-Moriya, and dipolar contributions has been obtained. In particular, we have proposed for the Neel skyrmion, a general ansatz for the magnetization component perpendicular to the dot, given by mz(r)=[1-(r/Rs)n]/[1+(r/Rs)n], where Rs is the radius of the skyrmion and n is an even integer number. As proof of concept, we calculate the energy of a Neel skyrmion in an ultra-thin Co/Pt cylinder, and we find that the dipolar contribution cannot be neglected and that both Dzyaloshinskii-Moriya interaction and anisotropy play an important role to stabilize the skyrmion. Additionally, we have obtained a good agreement between our analytical calculations and previously published micromagnetic simulations for n=10. For this reliable value of n, we have obtained that for a Dzyaloshinski Moriya constant D=5.5(mJ/m2), it is possible to stabilize a Neel skyrmion for Ku in the range 0.4(MJ/m3)<Ku<1.3(MJ/m3), whereas for Ku=0.8(MJ/m3), the skyrmion stabilizes for 5.0(mJ/m2)<D<6.0(mJ/m2). Thus, this analytical equation can be widely used to predict stability ranges for the Neel skyrmion in spintronic devices.

Determination of Radical-Radical Distances in Light-Active Proteins and Their Implication for Biological Magnetoreception.

Light-generated short-lived radial pairs have been suggested to play pivotal roles in cryptochromes and photolyases. Cryptochromes are very probably involved in magnetic compass sensing in migratory birds and the magnetic-field-dependent behavior of insects. We examined photo-generated transient states in the cryptochrome of Drosophila melanogaster and in the structurally related DNA-repair enzyme Escherichia coli DNA photolyase. Using pulsed EPR spectroscopy, the exchange and dipolar contributions to the electron spin-spin interaction were determined in a straightforward and direct way. With these parameters, radical-pair partners may be identified and the magnetoreceptor efficiency of cryptochromes can be evaluated. We present compelling evidence for an extended electron-transfer cascade in the Drosophila cryptochrome, and identified W394 as a key residue for flavin photoreduction and formation of a spin-correlated radical pair with a sufficient lifetime for high-sensitivity magnetic-field sensing.

Impact of the equation of state on calculated adsorption isotherm using DFT

In the early state of process development, usually high quality experimental data are often missing, especially, if the experimental effort is quite large. This situation occurs for the separation of very similar components, which must be separated applying adsorption. In principle, adsorption isotherms can be predicted using the density functional approach in combination with a suitable thermodynamic model in order to describe the fluid properties. In this paper, we study the adsorption of propanal, where no experimental data for comparison are available for verification of the modelling results. Therefore, we use three different equations of state (EOS), namely the Peng-Robinson and two versions out of the SAFT framework. The two versions are the Perturbed Chain – Statistical Association Fluid Theory (PC-SAFT) and the Perturbed Chain Polar – Statistical Association Fluid Theory (PCP-SAFT) including an additional dipole contribution. Although both SAFT versions are superior in modelling the phase behavior, especially the saturated liquid volume, the predicted adsorption isotherms were close together. However, the calculated condensation pressure in the pore depends on the chosen EOS. All equations of state lead to similar surface tensions, if they are coupled with the density gradient theory. The calculated surface tensions using one of the two SAFT versions are in excellent agreement with experimental data taken from the literature.

Polaron spin echo envelope modulations in an organic semiconducting polymer

Theoretical treatment of the electron spin echo envelope modulation (ESEEM) spectra from polarons in a semiconducting $\pi$- conjugated polymer is presented. The contact hyperfine coupling and the dipolar interaction between the polaron and proton spins are found to have distinct contributions in the ESEEM spectra. However, since the two contributions are spaced very closely, and the dipolar contribution is dominant, the detection of the contact hyperfine interaction is difficult. To resolve this problem, a recipe of probing the contact hyperfine and dipolar interactions selectively is proposed, and a method for detecting the polaron contact hyperfine interaction is formulated. The ESEEM decay due to the polaron random hopping is analyzed, and the robustness of the method against this decay is verified. Moreover, this decay is linked to the transport properties of polarons, providing an auxiliary probe for the polaron transport.

Magnetic micro-droplet in rotating field: numerical simulation and comparison with experiment

Magnetic droplets obtained by induced phase separation in a magnetic colloid show a large variety of shapes when exposed to an external field. However, the description of the shapes is often limited. Here, we formulate an algorithm based on three-dimensional boundary-integral equations for strongly magnetic droplets in a high-frequency rotating magnetic field, allowing us to find their figures of equilibrium in three dimensions. The algorithm is justified by a series of comparisons with known analytical results. We compare the calculated equilibrium shapes with experimental observations and find a good agreement. The main features of these observations are the oblate–prolate transition, the flattening of prolate shapes with the increase of magnetic field strength and the formation of starfish-like equilibrium shapes. We show both numerically and in experiments that the magnetic droplet behaviour may be described with a triaxial ellipsoid approximation. Directions for further research are mentioned, including the dipolar interaction contribution to the surface tension of the magnetic droplets, accounting for the large viscosity contrast between the magnetic droplet and the surrounding fluid.

Simultaneous dipole and quadrupole moment contribution in the Bogoliubov spectrum: Application of the non-integral Gross–Pitaevskii equation

We present the Gross–Pitaevskii equation for Bose–Einstein condensates (BECs) possessing the electric dipole and the electric quadrupole moments in a non-integral form. These equations are coupled with the Maxwell equations. The model under consideration includes the dipole–dipole, the dipole–quadrupole, and the quadrupole–quadrupole interactions in terms of the electric field created by the dipoles and quadrupoles. We apply this model to obtain the Bogoliubov spectrum for three-dimensional BECs with a repulsive short-range interaction. We obtain an extra term in the Bogoliubov spectrum in comparison with the dipolar BECs. We show that the quadrupole–quadrupole interaction gives a positive contribution in the Bogoliubov spectrum. Hence, this spectrum is stable.

Chemical bonding and nanomolecular length effects on work function at Au-organophosphonate-HfO2 interfaces

We demonstrate that introducing a thiol-terminated organophosphonate nanomolecular layer (NML) can increase the effective work function at Au-HfO2 interfaces by up to ΔΦeff = 0.55 ± 0.05 eV. Capacitance measurements of Au-NML-HfO2-SiO2-Si stacks and ultraviolet photoelectron spectroscopy of Au-NML-HfO2 structures, and parts thereof, reveal that Φeff shifts are primarily determined by the length of the molecules comprising the NML, while Au-NML and NML-oxide bonding dipole contributions tend to counteract each other. Our findings provide insights into tailoring the electronic properties of metal-oxide heterointerfaces for applications by harmonizing the effects of interfacial bonding and NML morphology.

Observation of the Isovector Giant Monopole Resonance via the ^{28}Si(^{10}Be,^{10}B^{*}[1.74 MeV]) Reaction at 100 AMeV.

The (^{10}Be,^{10}B^{*}[1.74 MeV]) charge-exchange reaction at 100 AMeV is presented as a new probe for isolating the isovector (ΔT=1) nonspin-transfer (ΔS=0) response of nuclei, with ^{28}Si being the first nucleus studied. By using a secondary ^{10}Be beam produced by fast fragmentation of ^{18}O nuclei at the NSCL Coupled Cyclotron Facility, applying the dispersion-matching technique with the S800 magnetic spectrometer to determine the excitation energy in ^{28}Al, and performing high-resolution γ-ray tracking with the Gamma-Ray Energy Tracking In-beam Nuclear Array (GRETINA) to identify the 1022-keV γ ray associated with the decay from the 1.74-MeV T=1 isobaric analog state in ^{10}B, a ΔS=0 excitation-energy spectrum in ^{28}Al was extracted. Monopole and dipole contributions were determined through a multipole-decomposition analysis, and the isovector giant dipole resonance and isovector giant monopole resonance (IVGMR) were identified. The results show that this probe is a powerful tool for studying the elusive IVGMR, which is of interest for performing stringent tests of modern density functional theories at high excitation energies and for constraining the bulk properties of nuclei and nuclear matter. The extracted distributions were compared with theoretical calculations based on the normal-modes formalism and the proton-neutron relativistic time-blocking approximation. Calculated cross sections based on these strengths underestimate the data by about a factor of 2, which likely indicates deficiencies in the reaction calculations based on the distorted wave Born approximation.

Sorption and Spatial Distribution of Protein Globules in Charged Hydrogel Particles.

We have theoretically studied the uptake of a nonuniformly charged biomolecule suitable for representing a globular protein or a drug by a charged hydrogel carrier in the presence of a 1:1 electrolyte. On the basis of the analysis of a physical interaction Hamiltonian including monopolar, dipolar, and Born (self-energy) contributions derived from linear electrostatic theory of the unperturbed homogeneous hydrogel, we have identified five different sorption states of the system, from complete repulsion of the molecule to its full sorption deep inside the hydrogel, passing through metastable and stable surface adsorption states. The results are summarized in state diagrams that also explore the effects of varying the electrolyte concentration, the sign of the net electric charge of the biomolecule, and the role of including excluded-volume (steric) or hydrophobic biomolecule-hydrogel interactions. We show that the dipole moment of the biomolecule is a key parameter controlling the spatial distribution of the globules. In particular, biomolecules with a large dipole moment tend to be adsorbed at the external surface of the hydrogel, even if like-charged, whereas uniformly charged biomolecules tend to partition toward the internal core of an oppositely charged hydrogel. Hydrophobic attraction shifts the states toward the internal sorption of the biomolecule, whereas steric repulsion promotes surface adsorption for oppositely charged biomolecules or for the total exclusion of likely charged ones. Our results establish a guideline for the spatial partitioning of proteins and drugs in hydrogel carriers, tunable by the hydrogel charge, pH, and salt concentration.

Impact of the dipole contribution on the terahertz emission of air-based plasma induced by tightly focused femtosecond laser pulses.

The present paper studies the generation mechanism of terahertz (THz) radiation from tightly focused femtosecond laser pulses in a gas medium. We measured the angular radiation pattern under different focusing conditions and observed that, with the deepening of focus, the angular radiation pattern changes and optical-to-THz conversion efficiency increases. The analysis of the observed phenomena led to the assumption that the dipole radiation prevails in most cases despite the existing conception regarding the dominating role of the quadrupole mechanism of radiation. Based on these assumptions, the transient photocurrent theory of the phenomenon presented in this paper was developed by us and used for the numerical fit of the experimental data.

Blueshift and phase tunability in planar THz metamaterials: the role of losses and toroidal dipole contribution.

We propose a model of tunable THz metamaterials. The main advantage is the blueshift of resonance and phase tunability due to inductive coupling in planar metallic metamolecules with incorporated silicon wires. We discuss the role of losses and toroidal dipole contribution to metamaterial response.

Atomic polarizations necessary for coherent infrared intensity modeling with theoretical calculations.

The inclusion of atomic polarizations for describing molecular electronic structure changes on vibration is shown to be necessary for coherent infrared intensity modeling. Atomic charges from the ChelpG partition scheme and atomic charges and dipoles from Quantum Theory of Atoms in Molecules (QTAIM) were employed within two different models to describe the stretching and bending vibrational intensities of the C-H, C-F, and C=O groups. The model employing the QTAIM parameters was the Charge-Charge Transfer and Dipolar Polarization model (QTAIM/CCTDP), and the model employing the ChelpG charges was the Equilibrium Charge-Charge Flux (ChelpG/ECCF). The QTAIM/CCTDP models result in characteristic proportions of the charge-charge transfer-dipolar polarization contributions even though their sums giving the total intensities do not discriminate between these vibrations. According to the QTAIM/CCTDP model, the carbon monoxide intensity has electronic structure changes similar to those of the carbonyl stretches whereas they resemble those of the CH stretches for the ChelpG/ECCF model.