Dipolar Contributions Research Articles

Performance of Magnetic Dipole Contribution on Electromagnetic Ellis Tetra Hybrid Nanofluid with the Applications of Surface Tension Gradient: A Xue Model Exploration

Performance of Magnetic Dipole Contribution on Electromagnetic Ellis Tetra Hybrid Nanofluid with the Applications of Surface Tension Gradient: A Xue Model Exploration

Synergistic contributions of the poling field-induced changes in local structure on the piezoelectric properties of modified BaTiO3 system

Abstract Local structural heterogeneity is a key factor in improving the piezoelectric properties of non-centrosymmetric piezoelectric systems. This work investigates electric field-induced structural and microstructural changes at localized and average scales to elucidate the structure-property correlations that enhance piezoelectric performance in Sn-doped BaTiO3 systems exhibiting coexisting phase boundaries. Despite showing field-induced structural phase transformation, the sample displays variations in piezocoefficient values with the nature of phase boundary compositions. Raman spectroscopy measurements reveal that the TiO6/SnO6 octahedra near the tetragonal-orthorhombic phase boundary exhibit significantly greater poling field-induced structural heterogeneities in local structure compared to those near the orthorhombic-cubic phase boundary. X-ray absorption spectroscopic results on Ti and Sn K-edge in unpoled and poled samples reveal that the dipolar contribution responsible for the piezoelectricity originates from field-induced distortion associated with both TiO6 and SnO6 octahedra. Near the vicinity of the tetragonal-orthorhombic phase boundary, both the TiO6 and SnO6 contributions are cumulative and exhibit better piezoelectricity. On the other hand, at the orthorhombic-cubic phase boundary, the dipolar contributions from these octahedra are counterintuitive, resulting in a reduction of piezoelectricity. These results could provide a pathway to design materials with an enhanced piezoelectric response by considering various phase boundary aspects before applying a poling field prior to making them piezoactive.

Microscopic view on the polarization-resolved S-SHG intensity of the vapor/liquid interface of pure water.

Second harmonic generation (SHG) is a nonlinear optical phenomenon where two photons at the frequency ω combine to form a single photon at the second-harmonic frequency 2ω. Since that second-order process is very weak in bulk isotropic media, optical SHG responses of interfaces provide a powerful and versatile technique to probe the molecular structure and dynamics of liquid interfaces. Both local dipole contributions and non-local quadrupole contributions can be interesting to investigate different properties of the interface, such as the molecular orientation or the charge density. However, a major difficulty is to comprehend the link between the S-SHG intensity and molecular details. This article reports a numerical approach to model the polarization-resolved SHG intensities of a model vapor/liquid interface of pure water. The influence of the interfacial local environment on the hyperpolarizability is taken into account using quantum mechanical/molecular mechanics calculations. The numerical predictions are in very good agreement with experiments. We detail the hypotheses made during the modeling steps and discuss the impact of various factors on the modeled SHG intensities, including the description of the exciting field in the interfacial layer, the effect of neighboring molecules on the second-harmonic polarization, and the presence of an additional static electric field at the interface.

Toroidal mode trapping in a magnetic meta-molecule

Abstract In this paper, we establish the relationship between the eigenmodes and the scattering characteristics of a meta-molecule made of magnetic disks from the point of view of the manifestation of its toroidal response. In particular, we examine the electric and magnetic dipole contributions to the scattering cross-sections obtained in the framework of the multipole decomposition method while accounting for the polarizability and magnetization induced in the structure by the field of incoming radiation. We find out that with increasing permeability, the toroidal mode is trapped in the meta-molecule due to the presence of its magnetization part, which may have a practical perspective in gyrotropy, permittivity, and permeability sensing.

Comprehensive constraints on fermionic dark matter-quark tensor interactions in direct detection experiments* *Supported in part by the Major Project of Basic and Applied Basic Research of Guangdong Province, China(2020B0301030008) and the National Natural Science Foundation of China(12035008, 12247151, 12305110, 12347121)

Effective field theory (EFT) provides a model-independent framework for interpreting the results of dark matter (DM) direct detection experiments. In this study, we demonstrate that the two fermionic DM-quark tensor operators and can contribute to the DM electric and magnetic dipole moments via nonperturbative QCD effects, in addition to the well-studied contact DM-nucleon operators. We then investigate the constraints on these two operators by considering both the contact and dipole contributions using the XENON1T nuclear recoil and Migdal effect data. We also recast other existing bounds on the DM dipole operators, derived from electron and nuclear recoil measurements in various direct detection experiments, as constraints on the two tensor operators. For , our results significantly extend the reach of constraints on the DM-quark tensor operators to masses as low as , with the bound exceeding that obtained by the Migdal effect with only contact interactions by approximately an order of magnitude. In particular, for the operator with DM mass , the latest PandaX constraint on the DM electric dipole moment puts more stringent bounds than the previous direct detection limit. We also briefly discuss the constraints obtained from experiments other than direct detection.

A new method to calculate broadband dielectric spectra of solvents from molecular dynamics simulations demonstrated with polarizable force fields.

Simulating the dielectric spectra of solvents requires the nuanced definition of inter- and intra-molecular forces. Non-polarizable force fields, while thoroughly benchmarked for dielectric applications, do not capture all the spectral features of solvents, such as water. Conversely, polarizable force fields have been largely untested in the context of dielectric spectroscopy but include charge and dipole fluctuations that contribute to intermolecular interactions. We benchmark non-polarizable force fields and the polarizable force fields AMOEBA03 and HIPPO for liquid water and find that the polarizable force fields can capture all the experimentally observed spectral features with varying degrees of accuracy. However, the non-polarizable force fields miss at least one peak. To diagnose this deficiency, we decompose the liquid water spectra from polarizable force fields at multiple temperatures into static and induced dipole contributions and find that the peak originates from induced dipole contributions. Broadening our inquiry to other solvents parameterized with the AMOEBA09 force field, we demonstrate good agreement between the experimental and simulated dielectric spectra of methanol and formamide. To produce these spectra, we develop a new computational approach to calculate the dielectric spectrum via the fluctuation dissipation theorem. This method minimizes the error in both the low and high frequency portions of the spectrum, improving the overall accuracy of the simulated spectrum and broadening the computed frequency range.

Second harmonic generation enhancement based on quasi-BICs in centrosymmetric materials

In centrosymmetric optical materials, the second-order nonlinear polarization of the bulk electric dipolar contribution is zero. More effective utilization of the contribution of the surface term is one of the key methods to efficiently obtain second-order nonlinear responses on these materials. Herein, a design of densely packed slotted nanopillar arrays based on quasi-bound states in the continuum (quasi-BICs) is proposed. The quasi-BICs are analyzed by using the finite element method as an example of silicon and the second harmonic generation (SHG) process is simulated. In the structure, normal-incidence linearly polarized light excites magnetic dipole-like quasi-BICs with a high quality factor which effectively promotes light-matter interactions. Increasing the nanopillar radius or decreasing the lattice constant within a certain range can cause the distribution of quality factors in k-space of the ky direction to contract toward the Γ point, which leads to a quasi-BIC with higher quality factors at the Γ point. By conjunctively adjusting the nanopillar radius and lattice constant or changing the slot azimuth, the resonance wavelength can be adjusted over a wide range (about several hundred nanometers) or finely (within about one nanometer) while maintaining high quality factors. When the symmetry perturbation introduced by the slot is small, it is calculated that the SHG conversion efficiency is about 10−6∼10−5 at an incident light power density of 1 MW/m2, and the SHG power is about 107∼108 times enhancement compared with the structure without slots. As the slot width decreases, higher SHG conversion efficiency with more significant SHG enhancement can be achieved at a specific slot length. The results provide new insights into the modulation of the resonant wavelength and quality factor of quasi-BICs, as well as the control of second-order nonlinear effects in centrosymmetric materials.

Inverse Faraday Effect in Ferrite–Garnet Films in the Near-Infrared Range

The magneto-optical Faraday effect is determined by the electric dipole and magnetic dipole transitions in a transparent magnetic material. At the same time, the inverse Faraday effect is still described by an expression that includes only electric dipole transitions. The magnetic dipole contribution to the inverse Faraday effect is considered theoretically, and the dependence of the inverse Faraday effect on the wavelength in the near-infrared range (where the magnetic dipole contribution becomes significant) is obtained by the example of a ferrite–garnet film. It is shown that, although both contributions to the inverse Faraday effect always take place for homogeneous films, only the magnetic-dipole inverse Faraday effect manifests itself for films with a periodic nanostructure upon excitation by a TE waveguide mode, which may be useful for its experimental observation.

Isomeric effects on the electron impact scattering for selected five membered heterocyclic ring molecules

We present electron scattering cross-sectional data for selected isomers of the five-membered ring molecules, specifically oxazole and isoxazole, thiazole and isothiazole, and imidazole and pyrazole. The ab-initio R-matrix method, incorporating static exchange polarization approximations, is employed for this calculation from energy range 0.1 eV to 20 eV. Three shape resonances are identified and characterized in each system, consisting of two π* and one σ* shape resonances. Notably, thiazole and isothiazole exhibit additional σ* resonance which is which is at a lower energy than other σ* resonance. The calculated resonance positions align well with available experimental as well as theoretical data. We also performed electronic structure calculations to aid in characterization of resonances. Comparison of the scattering cross-sectional data with their respective isomers reveal marginal differences in the magnitude of the elastic cross section particularly below 1 eV. This discrepancy may be attributed to variations in the long-range electronic dipole contribution to the electron-molecule interaction process. Further, to understand dependency of dipole moment on elastic cross section, we performed a fitting procedure for the elastic cross sections at 0.1 eV with square of the dipole moment of all the five membered ring molecules studied here. The fitting formula so obtained was used to estimate the cross section for other three five membered ring molecules: Furan, Thiophene and Pyrrole. Additionally, total ionization cross sections are computed using the binary-encounter-Bethe (BEB) model, demonstrating nearly identical results when compared with their isomers. Our findings offer insights into the influence of structural changes on the electron scattering data, providing guidance for other theoretical investigations.

Paramagnetic Properties of [AnIV(NO3)6]2- Complexes (An = U, Np, Pu) Probed by NMR Spectroscopy and Quantum Chemical Calculations.

Actinide +IV complexes with six nitrates [AnIV(NO3)6]2- (An = Th, U, Np, and Pu) have been studied by 15N and 17O NMR spectroscopy in solution and first-principles calculations. Magnetic susceptibilities were evaluated experimentally using the Evans method and are in good agreement with the ab initio values. The evolution in the series of the crystal field parameters deduced from ab initio calculations is discussed. The NMR paramagnetic shifts are analyzed based on ab initio calculations. Because the cubic symmetry of the complex quenches the dipolar contribution, they are only of Fermi contact origin. They are evaluated from first-principles based on a complete active space/density functional theory (DFT) strategy, in good accordance with the experimental one. The ligand hyperfine coupling constants are deduced from paramagnetic shifts and calculated using unrestricted DFT. The latter are decomposed in terms of the contribution of molecular orbitals. It highlights two pathways for the delocalization of the spin density from the metallic open-shell 5f orbitals to the NMR active nuclei, either through the valence 5f hybridized with 6d to the valence 2p molecular orbitals of the ligands, or by spin polarization of the metallic 6p orbitals which interact with the 2s-based molecular orbitals of the ligands.

Helmholtz energy models for dipole interactions: Review and comprehensive assessment

Dipolar interactions play an important role for thermodynamic properties of many fluids and accordingly for their modeling. In molecular-based equation of state models, the effect of dipolar interactions is usually described by Helmholtz energy models. There are several Helmholtz energy models for dipolar interactions available in the literature today. In this work, eight dipole contribution models describing the dipole–dipole interactions of fluids were critically assessed by comparing their results with molecular simulation reference data of Stockmayer fluids. Therefore, the dipole contribution models were combined with an accurate Lennard-Jones (LJ) Helmholtz energy model. The following thermodynamic properties were considered in the comparison: vapor pressure, saturated densities, enthalpy of vaporization, surface tension (by using density gradient theory), critical point, second virial coefficient, and thermodynamic properties at homogeneous state points, such as the Helmholtz energy, pressure, chemical potential, internal energy, isochoric heat capacity, isobaric heat capacity, thermal expansion coefficient, isothermal compressibility, thermal pressure coefficient, speed of sound, Joule–Thomson coefficient, and Grüneisen parameter. For the evaluation of the dipole contribution models, molecular simulations for the Stockmayer fluid with the dipole moments of μ2/4πϵ0ɛσ3=0.5,1,2,3,4,5 were carried out. The results indicate, that all considered dipole models exhibit some significant weaknesses. Nevertheless, some dipole contribution models are found to provide a robust description for many properties and state ranges. Overall, the deviations of the dipole contribution models from the Stockmayer simulation data are, in most cases, an order of magnitude higher than the deviations of the LJ EOS from LJ simulation data.

Broadband nonreciprocal gyromagnetic metasurface via magnetic Kerker-type dimers

Optical nonreciprocity, stemming from the deviation of the Lorentz reciprocity theorem, holds significant interest in the realm of optics and electromagnetics. Here, we propose and experimentally demonstrate broadband nonreciprocal transmission via a low-biased magnetic Kerker-type dimer metasurface. The designed magneto-optical metasurface comprises three layers of metal sandwiched between two gyromagnetic near-zero thickness slabs. The Kerker-type dimers broaden the isolation bandwidth utilizing multiple resonances where the double-stacked metallic disks act as Kerker-type dipoles, enhancing the transmissibility of the metasurface. The multipole decomposition reveals that the magnetic dipole contribution arising from magnetization is the primary cause of the metasurface's nonreciprocal response. Microwave measurement demonstrates that the bandwidth for an isolation ratio exceeding 10 dB is over 3 GHz. The broadband nonreciprocal performance remains relatively stable, exhibiting strong robustness against the bias disturbance. Our findings provide an alternative avenue for enhancing broadband nonreciprocity transmission under a low-biased magnetic field.

Influence of Quadrupolar Molecular Transitions within Plasmonic Cavities.

Optical nanocavities have revolutionized the manipulation of radiative properties of molecular and semiconductor emitters. Here, we investigate the amplified photoluminescence arising from exciting a dark transition of β-carotene molecules embedded within plasmonic nanocavities. Integrating a molecular monolayer into nanoparticle-on-mirror nanostructures unveils enhancements surpassing 4 orders of magnitude in the initially light-forbidden excitation. Such pronounced enhancements transcend conventional dipolar mechanisms, underscoring the presence of alternative enhancement pathways. Notably, Fourier-plane scattering spectroscopy shows that the photoluminescence excitation resonance aligns with a higher-order plasmonic cavity mode, which supports strong field gradients. Combining quantum chemistry calculations with electromagnetic simulations reveals an important interplay between the Franck-Condon quadrupole and Herzberg-Teller dipole contributions in governing the absorption characteristics of this dark transition. In contrast to free space, the quadrupole moment plays a significant role in photoluminescence enhancement within nanoparticle-on-mirror cavities. These findings provide an approach to access optically inactive transitions, promising advancements in spectroscopy and sensing applications.

Ambiguities in Decomposing Molecular Polarizability into Atomic Charge Flow and Induced Dipole Contributions.

The molecular dipole polarizability can be decomposed into components corresponding to the charge flow between atoms and changes in atomic dipole moments. Such decompositions are recognized to depend on how atoms are defined within a molecule, as, for example, by Hirshfeld, iterative Stockholder, or quantum topology partitioning of the electron density. For some of these, however, there are significant differences between the numerical results obtained by analytical response methods and finite field calculations. We show that this difference is due to analytical response methods accounting for (only) the change in electron density by a perturbation, while finite field methods may also include a component corresponding to a perturbation-dependent change in the definition of an atom within a molecule. For some atom-in-molecule definitions, such as the iterative Hirshfeld, iterative Stockholder, and quantum topology methods, the latter effect significantly increases the charge flow component. The decomposition of molecular polarizability into atomic charge flow and induced dipole components thus depends on whether the atom-in-molecule definition is taken to be perturbation-dependent.

Axionlike-particle contributions to the μ→e conversion

We study the μ→e conversion process in nuclear targets arising in models of axionlike particles (ALPs) with hadronic and charged lepton flavor violating (CLFV) interactions. Contributions to this process generally fall into two categories: spin-independent (SI) and spin-dependent (SD). While the SI contribution can be generated by a dipole operator through purely leptonic ALP interactions, the SD contribution can also be present through ALP-quark interactions at tree-level. It is naively anticipated that the SI contribution would be dominant due to its coherent enhancement. In this paper, we show that is not generically the case; in particular, for naturally sized ALP couplings to quarks of order ∼mq/fa, the SD interaction induced by ALP-π0 mixing turns out to be the leading contribution to μ→e conversion. Intuitively, this stems from the suppressed dipole contribution by the QED one-loop factor which counters the effect of SI coherent enhancement. Our study highlights the importance of μ→e conversion searches in exploring the parameter space of generic ALP models, and demonstrates the competitiveness of these searches in probing the CLFV ALP parameter space in the heavy mass range of ma≳mμ. Published by the American Physical Society 2024

On the monopolar and dipolar acoustic responses of a passive single point scatterer subjected to low-Mach-number grazing air flow

The acoustic response of a passive single point scatterer under grazing flow is shown theoretically and experimentally to have both monopolar and dipolar contributions. The monopolar response is dominated by the pressure-induced flux Qp, which is related to the specific acoustic impedance of the point scatterer as ζ=−1/Qp. By contrast, the main dipolar response is the pressure-induced force Fp, which is experimentally proven to be modelled by introducing a complex-valued factor η. In fact, η is related to the ratio between Qp and Fp. By employing these two complex-valued parameters ζ and η in the proposed theoretical transfer matrix model, the scattering properties of a single point scatterer (e.g., a Helmholtz resonator) subjected to grazing flow can be well predicted. This model can be readily used in practical applications such as the design of passive absorbers and silencers in ventilation systems.

Relativistic calculation of the orbital hyperfine splitting in complex microscopic structures

Theoretical spectroscopy based on double perturbation theory is typically challenged by systems with large orbital hyperfine splitting. Therefore, we here derive a rigorous, non-perturbative scheme starting from Dirac’s equation which allows to calculate the contribution of the orbital HFI for complex structures including heavy atoms with strong spin-orbit coupling (SOC). Using the PAW formalism, the method has been implemented in the software package Quantum ESPRESSO. We show that the ‘orbital part’ actually scales with SOC strength if orbital quenching is hindered by low local symmetry, i.e. in case of dimers or atoms at surfaces. This holds true in particular when the unpaired electron is localized in quasi-atomic p-like orbitals. Here, the orbital part is by far not negligible, but becomes dominant by surpassing the dipolar contribution by a factor of five.

Understanding Complex Interplay among Different Instabilities in Multiferroic BiMn7O12 Using 57Fe Probe Mössbauer Spectroscopy.

Here, we report the results of a Mössbauer study on hyperfine electrical and magnetic interactions in quadruple perovskite BiMn7O12 doped with 57Fe probes. Measurements were performed in the temperature range of 10 K < T < 670 K, wherein BiMn6.9657Fe0.04O12 undergoes a cascade of structural (T1 ≈ 590 K, T2 ≈ 442 K, and T3 ≈ 240 K) and magnetic (TN1 ≈ 57 K, TN2 ≈ 50 K, and TN3 ≈ 24 K) phase transitions. The analysis of the electric field gradient (EFG) parameters, including the dipole contribution from Bi3+ ions, confirmed the presence of the local dipole moments pBi, which are randomly oriented in the paraelectric cubic phase (T > T1). The unusual behavior of the parameters of hyperfine interactions between T1 and T2 was attributed to the dynamic Jahn-Teller effect that leads to the softening of the orbital mode of Mn3+ ions. The parameters of the hyperfine interactions of 57Fe in the phases with non-zero spontaneous electrical polarization (Ps), including the P1 ↔ Im transition at T3, were analyzed. On the basis of the structural data and the quadrupole splitting Δ(T) derived from the 57Fe Mössbauer spectra, the algorithm, based on the Born effective charge model, is proposed to describe Ps(T) dependence. The Ps(T) dependence around the Im ↔ I2/m phase transition at T2 is analyzed using the effective field approach. Possible reasons for the complex relaxation behavior of the spectra in the magnetically ordered states (T < TN1) are also discussed.

Comprehensive quantum calculation of the first dielectric virial coefficient of water.

We present a complete calculation, fully accounting for quantum effects and for molecular flexibility, of the first dielectric virial coefficient of water and its isotopologues. The contribution of the electronic polarizability is computed from a state-of-the-art intramolecular potential and polarizability surface from the literature, and its small temperature dependence is quantified. The dipolar polarizability is calculated in a similar manner with an accurate literature dipole-moment surface; it differs from the classical result both due to the different molecular geometries sampled at different temperatures and due to the quantization of rotation. We calculate the dipolar contribution independently from spectroscopic information in the HITRAN2020 database and find that the two methods yield consistent results. The resulting first dielectric virial coefficient provides a complete description of the dielectric constant at low density that can be used in humidity metrology and as a boundary condition for new formulations for the static dielectric constant of water and heavy water.

Magneto-plasmonic scattering by a disk-shaped particle made of an artificial dielectric

The main features of artificial dielectrics are high anisotropy and controllable heterogeneity, as well as adjustable values of their synthesized material parameters. In this work, we numerically study the scattering features of a disk-shaped particle made of an artificial dielectric (finely stratified structure, FSS) that is composed of magnetic and semiconductor constituents influenced by an external static magnetic field. The tensor-valued permittivity and permeability of the FSS are derived involving the effective medium theory. Due to a specific composition of the FSS, the material properties of the disk simultaneously acquire electric and magnetic gyrotropy, which depends on the proportion of the semiconductor and magnetic components included in the FSS. It is supposed that the ferromagnetic and plasma resonances of the constitutive materials are closely spaced. In particular, we examine the electric and magnetic dipole contributions to the scattering and absorption cross-sections obtained in the framework of the multipole decomposition method while accounting for the polarizability and magnetization induced in the particle by the field of incoming radiation. By varying the proportion of components of the artificial dielectric, we demonstrate the magneto-plasmonic functionality of the particle. Our presentation generalizes and complements several known solutions obtained separately for either magnetic or dielectric anisotropic particles. This approach can be used to study magneto-optical effects in metamaterials and metasurfaces composed of an ensemble of gyroelectric and gyromagnetic particles that is important for both plasmonic and photonic applications.