Temperature-induced local and average structural changes in BaTiO 3 - x Bi(Zn 1/2 Ti 1/2 )O 3 solid solutions: The origin of high temperature dielectric permittivity
Abstract not provided
Hou, Dong (ORCID:000000020942688X)↗
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Direct measurement of the static and transient magneto-optical permittivity of cobalt across the entire M -edge in reflection geometry by use of polarization scanning
The microscopic state of a magnetic material is characterized by its resonant magneto-optical response through the off-diagonal dielectric tensor component ε xy . However, the measurement of the full complex ε xy in the extreme ultraviolet spectral region covering the M absorption edges of 3d ferromagnets is challenging due to the need for either a careful polarization analysis, which is complicated by a lack of efficient polarization analyzers, or scanning the angle of incidence in fine steps. Here, we propose and demonstrate a technique to extract the complex resonant permittivity ε xy simply by scanning the polarization angle of linearly polarized high harmonics to measure the magneto-optical asymmetry in reflection geometry. Because this technique is more practical and faster to experimentally implement than previous approaches, we can directly measure the full time evolution of ε xy (t) during laser-induced demagnetization across the entire M 2,3 absorption edge of cobalt with femtosecond time resolution. We find that for polycrystalline Co films on an insulating substrate, the changes in ε xy are uniform throughout the spectrum, to within our experimental precision. This result suggests that, in the regime of strong demagnetization, the ultrafast demagnetization response is primarily dominated by magnon generation. Here, we estimate the contribution of exchange-splitting reduction to the ultrafast demagnetization process to be no more than 25%.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
The permittivity and refractive index measurements of doped barium titanate (BT-BCN)
Not Available
Meeker, Michael A.↗
Permittivity Threshold and Thermodynamics of Integer Charge-Transfer Complexation for an Organic Donor–Acceptor Pair
Molecular or chemical-based charge doping provides a means to change the properties (e.g. conductivity) of a material through a complete or partial transfer of charge between its constituents. Understanding how local material environment impacts this process is thus important for controlling the properties of organic materials. This paper presents spectroscopic investigations of molecular charge transfer interactions between a pair of common charge-doping and -transporting materials (2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane, F4TCNQ, and N,N’-Diphenyl-N-N’-di-p-tolylbenzene-1,4-diamine, MPDA). Equilibrium constants associated with charge transfer were determined for donor-acceptor pairs dissolved in a series of solvents covering a range of values of permittivity. A threshold for highly favorable charge separation was observed to occur at a permittivity of ~8-9, with more and less favorable charge separation observed in solvents of higher and lower permittivity, respectively, but with chloroform (permittivity=4.81) exhibiting an anomalously favorable charge separation. Temperature-dependent studies were undertaken to assess the thermodynamics of charge separation. In 1,2- dichloroethane (permittivity=10.36) and chlorobenzene (permittivity=5.62), charge transfer was observed to be both enthalpically and entropically favorable. Charge separation in chloroform is exothermic and entropically disfavored, indicating that specific, inner-shell solvent-solute interactions stabilize the charge-separated complex and result in a net increase in local solution structure. Furthermore, our results provide insight on how modification to the chemical environment may be utilized to support stable charge transfer for molecular doping applications and requiring only modest changes in local permittivity.
36 MATERIALS SCIENCE↗
Multiscale modeling of packed-bed microwave reactors and estimation of intrinsic materials' permittivity
Modeling of packed-bed microwave reactors relies on an accurate representation of particle size, shape, and distribution within the bed, as well as the particles' dielectric properties. The measured permittivity of microwave susceptors (powders or structured materials) depends on the geometric features of the particles and the porosity of the bed, as well as the specific form factor of a structured material. These are effective properties and cannot be used to analyze other reactor configurations unless the geometric effects are removed. Therefore, we introduce a methodology for extracting the intrinsic particle permittivity from experimentally measured effective permittivity by combining cavity-based measurements with multiscale simulations and machine learning. Further, we develop the first multiscale model of packed-bed microwave reactors that incorporate particle effects (geometric features, random packing, and particle contact). This approach bridges macroscopic observables with mesoscopic physics, enabling analysis of local hotspots, arcing, and contact effects that control reactor performance. Using polymer-based spherical activated carbon (PBSAC) and silicon carbide (SiC) as examples, we demonstrate that the inferred particle permittivity is consistent with independent experimental heating profiles we collect from microwave reactors without adjustable parameters. Finally, this methodology establishes a foundation for predictive, multiscale design of microwave packed-bed reactors that explicitly accounts for particle-scale effects, enabling the estimation of intrinsic permittivity for the first time.
97 MATHEMATICS AND COMPUTING↗
Precision measurement of relative permittivity of aluminum oxide for a high power resonant waveguide window with low return loss
An iterative method of estimating permittivity and window thickness with high precision is developed for half wavelength resonant waveguide windows for use in a lower hybrid launcher for DIII-D. The high Q factor of half-wavelength windows results in extreme sensitivity of return loss on small deviations in permittivity. Permittivity and loss tangent measurements of Morgan AL-995 99.5% aluminum oxide ceramic using a waveguide resonant cavity per ASTM D2520-13 determine variation of permittivity with frequency. Measurement of window resonant frequency in conjunction with the slope of permittivity from waveguide cavity measurements determine required thickness of a resonant window within 5 MHz of the desired resonant frequency. Methods to improve measurement accuracy of resonant peaks on a vector network analyzer are discussed. A sensitivity study to dimensional variations in window or sample rod geometry, and shift in resonant frequency due to RF heating of the window material is conducted.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Extraordinarily large permittivity modulation in zinc oxide for dynamic nanophotonics
The dielectric permittivity of a material encapsulates the essential physics of light-matter interaction into the material's local response to optical excitation. Photo-induced modulation of the permittivity can enable an unprecedented level of control over the phase, amplitude, and polarization of light. Therefore, the detailed dynamic characterization of technology-relevant materials with substantially tunable optical properties and fast response times is a crucial step to realize tunable optical devices. This work reports on the extraordinarily large permittivity changes in zinc oxide thin films (up to similar to 3.6 relative change in the real part of the dielectric permittivity at 1600 nm wavelength) induced by optically generated free carriers. We demonstrate broadband reflectance modulation up to 70% in metal-backed oxide mirrors at the telecommunication wavelengths, with picosecond-scale relaxation times. The epsilon near zero points of the films can be dynamically shifted from 8.5 mm to 1.6 mm by controlling the pump fluence. Additionally, the modulation can be selectively enhanced at specific wavelengths employing metal-backed zinc oxide disks while maintaining picosecond-scale switching times. This work provides insights into the free-carrier assisted permittivity modulation in zinc oxide and could enable the realization of novel dynamic devices for beam-steering, polarizers, and spatial light modulators.
36 MATERIALS SCIENCE↗
Ion Pairing and Redissociaton in Low-Permittivity Electrolytes for Multivalent Battery Applications
Detailed speciation of electrolytes as a function of chemical system and concentration provides the foundation for understanding bulk transport as well as possible decomposition mechanisms. In particular, multivalent electrolytes have shown a strong coupling between anodic stability and solvation structure. Furthermore, solvents that are found to exhibit reasonable stability against alkaline-earth metals generally exhibit low permittivity, which typically increases the complexity of the electrolyte species. To improve our understanding of ionic population and associated transport in these important classes of electrolytes, the speciation of Mg(TFSI)2 in monoglyme and diglyme systems is studied via a multiscale thermodynamic model using first-principles calculations for ion association and molecular dynamics simulations for dielectric properties. The results are then compared to Raman and dielectric relaxation spectroscopies, which independently confirm the modeling insights. We find that the significant presence of free ions in the low-permittivity glymes in the concentration range from 0.02 to 0.6 M is well-explained by the low-permittivity redissociation hypothesis. Here, salt speciation is largely dictated by long-range electrostatics, which includes permittivity increases due to polar contact ion pairs. The present results suggest that other low-permittivity multivalent electrolytes may also reach high conductivities as a result of redissociation.
25 ENERGY STORAGE↗
Percolative NiO decorated reduced-graphene oxide with a giant dielectric permittivity
Highlights: • NiO/r-GO composite exhibited a gaint dielectric permittivity of 3688 at 1 kHz. • NiO/r-GO composite is percolative w.r.t dielectric permittivity and conductivity. • Low threshold percolation is observed. • Increasing r-GO wt% decreased the interfacial resistance consistent with conductivity variation. - Abstract: NiO decorated reduced graphene oxide (r-GO) composites with varying r-GO weight percentages are synthesized using molecular level mixing technique. These composites are found to follow percolation theory with respect to dielectric behavior and conductivity values. A giant permittivity (ε′) value of 3688 was measured at 1 kHz when 2.4 wt% of r-GO was used in preparing NiO/r-GO composite. In comparison to NiO, enhanced permittivity values are recorded in the case of NiO/r-GO composites due to Maxwell-Wagner interfacial polarization between functionalized graphene sheets and NiO particles. It was also observed that ε′ values increased with decreasing NiO grain size up to the percolation threshold value. Moreover, ε′ values are found to be consistent with universal threshold values. Cole–Cole plots’ analysis revealed that the interfaces in the composites are more active than NiO grains.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Excitation and propagation of surface plasmon polaritons on a non-structured surface with a permittivity gradient
Accompanied by the rise of plasmonic materials beyond those based on noble metals and the development of advanced materials processing techniques, it is important to understand the plasmonic behavior of materials with large-scale inhomogeneity (such as gradient permittivity materials) because they cannot be modeled simply as scatterers. In this paper, we theoretically analyze the excitation and propagation of surface plasmon polaritons (SPPs) on a planar interface between a homogeneous dielectric and a material with a gradient of negative permittivity. We demonstrate the following: (i) free-space propagating waves and surface waves can be coupled by a gradient negative-permittivity material and (ii) the coupling can be enhanced if the material permittivity variation is suitably designed. This theory is then verified by numerical simulations. A direct application of this theory, ‘rainbow trapping’, is also proposed, considering a realistic design based on doped indium antimonide. This theory may lead to various applications, such as ultracompact spectroscopy and dynamically controllable generation of SPPs.
36 MATERIALS SCIENCE↗
Why Dissolving Salt in Water Decreases Its Dielectric Permittivity
The dielectric permittivity of salt water decreases on dissolving more salt. For nearly a century, this phenomenon has been explained by invoking saturation in the dielectric response of the solvent water molecules. Herein, we employ an advanced deep neural network (DNN), built using data from density functional theory, to study the dielectric permittivity of sodium chloride solutions. Notably, the decrease in the dielectric permittivity as a function of concentration, computed using the DNN approach, agrees well with experiments. Detailed analysis of the computations reveals that the dominant effect, caused by the intrusion of ionic hydration shells into the solvent hydrogen-bond network, is the disruption of dipolar correlations among water molecules. Accordingly, the observed decrease in the dielectric permittivity is mostly due to increasing suppression of the collective response of solvent waters.
74 ATOMIC AND MOLECULAR PHYSICS↗
Local negative permittivity and topological phase transition in polar skyrmions
Topological solitons such as magnetic skyrmions have drawn attention as stable quasi-particle-like objects. The recent discovery of polar vortices and skyrmions in ferroelectric oxide superlattices has opened up new vistas to explore topology, emergent phenomena and approaches for manipulating such features with electric fields. Using macroscopic dielectric measurements, coupled with direct scanning convergent beam electron diffraction imaging on the atomic scale, theoretical phase-field simulations and second-principles calculations, we demonstrate that polar skyrmions in (PbTiO 3 ) n /(SrTiO 3 ) n superlattices are distinguished by a sheath of negative permittivity at the periphery of each skyrmion. This enhances the effective dielectric permittivity compared with the individual SrTiO 3 and PbTiO 3 layers. Moreover, the response of these topologically protected structures to electric field and temperature shows a reversible phase transition from the skyrmion state to a trivial uniform ferroelectric state, accompanied by large tunability of the dielectric permittivity. Pulsed switching measurements show a time-dependent evolution and recovery of the skyrmion state (and macroscopic dielectric response). The interrelationship between topological and dielectric properties presents an opportunity to simultaneously manipulate both by a single, and easily controlled, stimulus, the applied electric field. Polar skyrmions are topologically protected structures that can exist in (PbTiO 3 ) n /(SrTiO 3 ) n superlattices. Here, it is shown that they have negative permittivity at the surface, and that they can undergo a reversible phase transition with large dielectric tunability under an electric field.
36 MATERIALS SCIENCE↗
Origin of colossal dielectric permittivity of rutile Ti 0.9 In 0.05 Nb 0.05 O 2 : single crystal and polycrystalline
Here in this article, we investigated the dielectric properties of (In + Nb) co-doped rutile TiO 2 single crystal and polycrystalline ceramics. Both of them showed colossal, up to 10 4 , dielectric permittivity at room temperature. The single crystal sample showed one dielectric relaxation process with a large dielectric loss. The voltage-dependence of dielectric permittivity and the impedance spectrum suggest that the high dielectric permittivity of single crystal originated from the surface barrier layer capacitor (SBLC). The impedance spectroscopy at different temperature confirmed that the (In+Nb) co-doped rutile TiO 2 polycrystalline ceramic had semiconductor grains and insulating grain boundaries, and that the activation energies were calculated to be 0.052 eV and 0.35 eV for grain and grain boundary, respectively. The dielectric behavior and impedance spectrum of the polycrystalline ceramic sample indicated that the internal barrier layer capacitor (IBLC) mode made a major contribution to the high ceramic dielectric permittivity, instead of the electron-pinned defect-dipoles.
36 MATERIALS SCIENCE↗
Mimicking surface polaritons for unpolarized light with high-permittivity materials
Tailoring near-field optical phenomena often requires excitation of surface plasmon polaritons (SPPs) or surface phonon polaritons (SPhPs), surface waves at the interface between media with electric permittivities of opposite sign. Despite their unprecedented field confinement, surface polaritons are limited by polarization: only transverse magnetic fields enable their excitation, leaving transverse electric fields unexploited. By contrast, guided modes in positive permittivity materials occur for both linear polarizations, however, they typically cannot compete with SPPs and SPhPs in terms of confinement. Furthermore we show that omnipolarization guided modes in materials with high-permittivity resonances can reach confinement factors similar to SPPs and SPhPs, while surpassing them in terms of propagation distance. We explore the cases of silicon carbide and transition-metal dichalcogenides near their permittivity resonances, and compare with SPhPs in silicon carbide and SPPs in silver, at infrared and visible frequencies, respectively.
36 MATERIALS SCIENCE↗
A General Strategy to Achieve Colossal Permittivity and Low Dielectric Loss Through Constructing Insulator/Semiconductor/Insulator Multilayer Structures
In this work, we propose a route to realize high-performance colossal permittivity (CP) by creating multilayer structures of insulator/semiconductor/insulator. To prove the new concept, we made heavily reduced rutile TiO{sub 2} via annealing route in Ar/H{sub 2} atmosphere. Dielectric studies show that the maximum dielectric permittivity (~ 3.0 × 10{sup 4}) of our prepared samples is about 100 times higher than that (~ 300) of conventional TiO{sub 2}. The minimum dielectric loss is 0.03 (at 10{sup 4}–10{sup 5} Hz). Furthermore, CP is almost independent of the frequency (100–10{sup 6} Hz) and the temperature (20–350 K). We suggest that the colossal permittivity is attributed to the high carrier concentration of the inner TiO{sub 2} semiconductor, while the low dielectric loss is due to the presentation of the insulator layer on the surface of TiO{sub 2}. The method proposed here can be expanded to other material systems, such as semiconductor Si sandwiched by top and bottom insulator layers of Ga{sub 2}O{sub 3}.
36 MATERIALS SCIENCE↗
Indirect morphological analysis of particles in polymer particle composites via non-destructive permittivity measurements
We report polymers with specific properties (e.g. electrical, optical or mechanical) are commonly obtained via the addition of additives. The composites final properties rely on the preservation of these additives during embedding, which is, in particular, challenging for high aspect ratio particles, like shear-sensitive flaky particles (ssFP). Thus, in cases of ssFP off- or in-line monitoring is required. This study addresses the lack of suitable non-destructive monitoring methods appropriate for ssFP possessing a thickness below 1um and an area equivalent diameter of several 10 um. An elegant method was developed to validate the integrity of ssFP within composites, which is based on the measurement of the composite's permittivity and applying precise micro-structure property correlations to indirectly determine their morphological features. The main hypothesis tested was that a reduction of the particle’s aspect ratio by a factor of larger than 5 can be detected by the measurement of the composite's permittivity. In this study,the matrix polymer polyethylene or an epoxy resin together with mica-based ssFP with a mean area equivalent diameter of 42 um were used. The micro-structure property correlation presented by G. Ondracek [Z. f. Werkstofftechnik, 8:280-287, 1977] provided the necessary theoretical backbone to indirectly infer geometrical changes to the ssFP from permittivity measurements. An excellent match was obtained between the indirectly and the directly determined particle aspect ratios. This preliminary study established the presented technique as a promising non-destructive test method to monitor the integrity of ssFPs embedded in a polymer. In principle this technique is adaptable for in-line process monitoring.
36 MATERIALS SCIENCE↗
The effect of BaTiO{sub 3} particle shape on complex permittivity of 0.98MgTiO{sub 3}–0.02BaTiO{sub 3} composite powders at GHz frequencies
Highlights: • Elongated micrometre sized BaTiO{sub 3} particles had strong effect on permittivity. • Effect was significantly stronger compared to μm and nm sized spherical particles. • Properties could be tailored by varying the particle shapes of dielectric powders. • Could be utilized, e.g., in a production of electrical composites for RF applications. - Abstract: The effect of BaTiO{sub 3} particle shape on the properties of 0.98MgTiO{sub 3}–0.02BaTiO{sub 3} composite powders was characterized and analyzed using an indirectly coupled open-ended coaxial cavity resonator at gigahertz frequencies. Elongated micrometre sized BaTiO{sub 3} particles were found to have a significantly stronger effect on permittivity when compared to composite powders having micro and nano sized spherical BaTiO{sub 3} particles. Inclusion permittivities and dielectric loss tangents of composite powders increased from that of pure MgTiO{sub 3} powder, 13.3 and 4.6 × 10{sup −3}, up to 15.7 and 1.7 × 10{sup −2} with needle shaped BaTiO{sub 3} particles, respectively. The presented results give valuable information for tailoring the properties of dielectrics which can be utilized in the vast field of electronic component manufacturing.
36 MATERIALS SCIENCE↗