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At least 667 records · Page 37

Exploiting universal nonlocal dispersion in optically active materials for spectro-polarimetric computational imaging

Recent years have seen significant advancements in exploring novel light-matter interactions such as hyperbolic dispersion within natural crystals. However, current studies have predominantly concentrated on local optical response of materials characterized by a dielectric tensor without spatial dispersion. Here, we investigate the nonlocal response in optically-active crystals with screw symmetries, revealing their lossless, super-dispersive properties compared to traditional optical response functions. We leverage this universal nonlocal dispersion, i.e. the dispersion of optical rotatory power, to explore a novel spectral de-multiplexing scheme compared to conventional gratings, prisms and metasurfaces. We design and demonstrate an ‘Nonlocal-Cam’ - a camera that exploits nonlocal dispersion through sampling of polarized spectral states and the application of computational spectral reconstruction algorithms. The Nonlocal-Cam captures information in both laboratory and outdoor field experiments which is unavailable to traditional intensity cameras - the spectral texture of polarization. Merging the fields of nonlocal electrodynamics and computational imaging, our work paves the way for exploiting nonlocal optics of optically active materials in a variety of applications, from biological microscopy to physics-driven machine vision and remote sensing.

Wang, Xueji [Purdue Univ., West Lafayette, IN (Uni↗

Acceptor dopant mediated electrical property modification in Bi0.5Na0.5TiO3-based piezoceramic

The effect of Mn and Fe dopants on the electromechanical and electrochemical properties of 0.88[Bi 0.5 Na 0.5 ]TiO 3 –0.08[Bi 0.5 K 0.5 ]TiO 3 –0.04[Bi 0.5 Li 0.5 ]TiO 3 piezoceramic is investigated with particular emphasis on complex impedance in the temperature range from 450 to 600 °C. The impedance spectra have been simulated with equivalent circuits in order to extract bulk and grain boundary characteristics and to determine activation energies of conduction. Mn and Fe dopants considerably enhance the mechanical quality factor and decrease the dielectric loss compared to the undoped composition. Mn doping leads to dramatically higher resistivity in the bulk and a modest increase in the bulk activation energy. On the other hand, conductivity increases dramatically via Fe doping with a significant lowering of activation energy in the bulk and corresponding raising of the activation energy at grain boundaries in comparison to Mn-doped and undoped ceramic. The bulk conductivity of Fe-doped piezoceramic reaches as high as 0.01 S cm -1 at 600 °C.

36 MATERIALS SCIENCE↗

Ab Initio Prediction of Ultra‐Wide Band Gap B x Al 1− x N Materials

Abstract Ultra‐wide bandgap (UWBG) materials are poised to play an important role in the future of power electronics. Devices made from UWBG materials are expected to operate at higher voltages, frequencies, and temperatures than current silicon and silicon‐carbide‐based devices and can even lead to significant miniaturization of such devices. In the UWBG field, aluminum nitride and boron nitride have attracted great interest; however, the B x Al 1− x N alloys are much less studied. In this work, using first‐principles simulations combining density‐functional theory and the cluster expansion method, the crystal structure of B x Al 1− x N alloys is predicted. Seventeen ground state structures of B x Al 1− x N with formation energies between 0.11 and 0.25 eV atom ‐1 are found. All of these structures are found to be dynamically stable. The B x Al 1− x N structures are found to have predominantly a tetrahedral bonding environment; however, some structures exhibit sp 2 bonds similar to hexagonal BN. This work expands knowledge of the structures, energies, and bonding in B x Al 1− x N which aids their synthesis, the innovation of lateral or vertical devices, and discovery of compatible dielectric and Ohmic contact materials.

36 MATERIALS SCIENCE↗

The nature of the subsurface of Mercury from microwave observations at several wavelengths

Interferometric observations of Mercury at 3.71 cm are used to determine the dielectric constant of the subsurface material at a depth of 50 cm to be 2.4 plus or minus 0.3. The surface emissivity in the radio range is determined by the value of the dielectric constant which is thus necessary in order to interpret the thermal properties of the regolith. New integrated-disk data at 6- and 18-cm wavelengths are found to be consistent with a regolith of particulate geological material in which radiative transfer of heat is important. The results are very similar to the lunar case where regolith density, dielectric constant, and loss tangent are observed to increase smoothly with depth in the subsurface.

Cuzzi, J. N.↗

First-principles study of an S = 1 quasi one-dimensional quantum molecular magnetic material

We use density functional theory to study the structural, magnetic, and electronic structures of the organometallic quantum magnet NiCl 2-4 SC (NH 2 ) 2 (DTN). Recent work has demonstrated the quasi one-dimensional nature of the molecular crystal and studied its quantum phase transitions at low temperatures. The system includes a magnetoelectric (ME) coupling and, when doped with Br, the presence of an exotic Bose-glass state. Using the generalized gradient approximation with inclusion of a van der Waals term to account for weak intermolecular forces and by introducing a Hubbard U term to the total energy, we systematically show that our calculations reproduce the magnetic anisotropy, the intermolecular exchange coupling strength, and the magnetoelectric effect in DTN, which have been observed in previous experiments. Further analysis of the electronic structure gives insight into the underlying magnetic interactions, including what mechanisms may be causing the ME effect. Using this computationally efficient model, we predict what effect applying an electric field might have on the magnetic properties of this quantum magnet.

1-dimensional spin chains↗

Electrical Capacitance Volume Tomography for the Packed Bed Reactor ISS Flight Experiment

Fixed packed bed reactors are compact, require minimum power and maintenance to operate, and are highly reliable. These features make this technology a highly desirable unit operation for long duration life support systems in space. NASA is developing an ISS experiment to address this technology with particular focus on water reclamation and air revitalization. Earlier research and development efforts funded by NASA have resulted in two hydrodynamic models which require validation with appropriate instrumentation in an extended microgravity environment. To validate these models, the instantaneous distribution of the gas and liquid phases must be measured.Electrical Capacitance Volume Tomography (ECVT) is a non-invasive imaging technology recently developed for multi-phase flow applications. It is based on distributing flexible capacitance plates on the peripheral of a flow column and collecting real-time measurements of inter-electrode capacitances. Capacitance measurements here are directly related to dielectric constant distribution, a physical property that is also related to material distribution in the imaging domain. Reconstruction algorithms are employed to map volume images of dielectric distribution in the imaging domain, which is in turn related to phase distribution. ECVT is suitable for imaging interacting materials of different dielectric constants, typical in multi-phase flow systems. ECVT is being used extensively for measuring flow variables in various gas-liquid and gas-solid flow systems. Recent application of ECVT include flows in risers and exit regions of circulating fluidized beds, gas-liquid and gas-solid bubble columns, trickle beds, and slurry bubble columns. ECVT is also used to validate flow models and CFD simulations. The technology is uniquely qualified for imaging phase concentrations in packed bed reactors for the ISS flight experiments as it exhibits favorable features of compact size, low profile sensors, high imaging speed, and flexibility to fit around columns of various shapes and sizes. ECVT is also safer than other commonly used imaging modalities as it operates in the range of low frequencies (1 MHz) and does not radiate radioactive energy. In this effort, ECVT is being used to image flow parameters in a packed bed reactor for an ISS flight experiment.

Tomography↗

Joint inversion of electromagnetic measurements for the determination of water saturation profiles in concrete structures

Highlights: • DC-electrical and dielectric data are combined to estimate concrete saturation degree. • A joint inversion approach of the electromagnetic measurements is proposed. • The sensitivity of the measurements to the saturation model parameters is analysed. • The new joint approach was developed and is applied to synthetic and real data. • The benefits of the joint approach over the inversion of one data type are highlighted. Water saturation profiles in concrete are essential to assess its durability and can be determined using non-destructive techniques, especially the electric and the capacitive methods. In this paper, we propose a new inversion scheme where both resistivity and permittivity measurements are inverted jointly to retrieve the saturation profile. The finite element method is used to model the measurements in 3D, the concrete having a saturation profile with depth, represented by a continuous model taking the form of a Weibull curve with four parameters. A non-linear least-squares optimization based on the Levenberg-Marquardt scheme is developed for the inversion of measurements. Results show that information gathered from both measurements enriches the reconstructed profile, leading to a more reliable estimation of saturation profiles. We believe that the joint inversion method herein developed could lead to the study of more complex phenomena, such as the coupled water-chloride ingress.

36 MATERIALS SCIENCE↗

Uniqueness of relaxation times determined by dielectric spectroscopy

Dielectric spectroscopy is extremely powerful to study molecular dynamics, because of the very broad frequency range. Often multiple processes superimpose resulting in spectra that expand over several orders of magnitude, with some of the contributions partially hidden. For illustration, we selected two examples, (i) normal mode of high molar mass polymers partially hidden by conductivity and polarization and (ii) contour length fluctuations partially hidden by reptation using the well-studied polyisoprene melts as example. The intuitive approach to describe experimental spectra and to extract relaxation times is the addition of two or more model functions. Here, we use the empirical Havriliak-Negami function to illustrate the ambiguity of the extracted relaxation time, despite an excellent agreement of the fit with experimental data. We show that there are an infinite number of solutions for which a perfect description of experimental data can be achieved. However, a simple mathematical relationship indicates uniqueness of the pairs of the relaxation strength and relaxation time. Sacrificing the absolute value of the relaxation time enables to find the temperature dependence of the parameters with a high accuracy. For the specific cases studied here, the time temperature superposition (TTS) is very useful to confirm the principle. However, the derivation is not based on a specific temperature dependence, hence, independent from the TTS. We compare new and traditional approaches and find the same trend for the temperature dependence. The important advantage of the new technology is the knowledge of the accuracy of the relaxation times. Relaxation times determined from data for which the peak is clearly visible are the same within the experimental accuracy for traditional and new technology. However, for data where a dominant process hides the peak, substantial deviations can be observed. Finally, we conclude that the new approach is particularly helpful for cases in which relaxation times need to be determined without having access to the associated peak position.

36 MATERIALS SCIENCE↗

Preliminary Evaluation of Polyarylate Dielectric Films for Cryogenic Applications

Polymeric materials are used extensively on spacecraft and satellites in electrical power and distribution systems, as thermal blankets and optical surface coatings, as well as mechanical support structures. The reliability of these systems when exposed to the harsh environment of space is very critical to the success of the mission and the safety of the crew in manned-flight ventures. In this work, polyarylate films were evaluated for potential use as capacitor dielectrics and wiring insulation for cryogenic applications. Two grades of the film were characterized in terms of their electrical and mechanical properties before and after exposure to liquid nitrogen (-196 C). The electrical characterization consisted of capacitance and dielectric loss measure Cents in the frequency range of 50 Hz to 100 kHz, and volume and surface resistivities. The mechanical measurements performed included changes in tensile (Young's modulus, elongation-at-break, and tensile strength) and structural properties (dimensional change, weight, and surface morphology). The preliminary results, which indicate good stability of the polymer after exposure to liquid nitrogen, are presented and discussed.

Patterson, Richard L.↗

A Many-Body Perturbation Theory Approach to Energy Band Alignment at the Crystalline Tetracene–Silicon Interface

Hybrid inorganic–organic semiconductor (HIOS) interfaces are of interest for new photovoltaic devices operating above the Shockley–Queisser limit. Predicting energy band alignment at the interfaces is crucial for their design, but represents a challenging problem due to the large scales of the system, the energy precision required and a wide range of physical phenomena that occur at the interface. To tackle this problem, many-body perturbation theory in the non-self-consistent GW approximation, orbital relaxation corrections for organic semiconductors, and line-up potential method for inorganic semiconductors which allows for tractable and accurate computing of energy band alignment in crystalline van-der-Waals hybrid inorganic–organic semiconductor interfaces are used. In this work, crystalline tetracene physisorbed on the clean hydrogen-passivated 1 × 2 reconstructed (100) silicon surface is studied. Using this computational approach, it is found that the energy band alignment is determined by an interplay of the mutual dynamic dielectric screening of two materials and the formation of a dipole layer due to a weak hybridization of atomic/molecular orbitals at the interface. The significant role of the exchange-correlation effects in predicting band offsets for the hybrid inorganic–organic semiconductor interfaces is also emphasized.

74 ATOMIC AND MOLECULAR PHYSICS↗

Chemical Profiles of the Oxides on Tantalum in State of the Art Superconducting Circuits

Abstract Over the past decades, superconducting qubits have emerged as one of the leading hardware platforms for realizing a quantum processor. Consequently, researchers have made significant effort to understand the loss channels that limit the coherence times of superconducting qubits. A major source of loss has been attributed to two level systems that are present at the material interfaces. It is recently shown that replacing the metal in the capacitor of a transmon with tantalum yields record relaxation and coherence times for superconducting qubits, motivating a detailed study of the tantalum surface. In this work, the chemical profile of the surface of tantalum films grown on c‐plane sapphire using variable energy X‐ray photoelectron spectroscopy (VEXPS) is studied. The different oxidation states of tantalum that are present in the native oxide resulting from exposure to air are identified, and their distribution through the depth of the film is measured. Furthermore, it is shown how the volume and depth distribution of these tantalum oxidation states can be altered by various chemical treatments. Correlating these measurements with detailed measurements of quantum devices may elucidate the underlying microscopic sources of loss.

36 MATERIALS SCIENCE↗

Dynamic control of ferroionic states in ferroelectric nanoparticles

The polar states of uniaxial ferroelectric nanoparticles interacting with a surface system of electronic and ionic charges with a broad distribution of mobilities is explored, which corresponds to the experimental case of nanoparticles in solution or ambient conditions. The nonlinear interactions between the ferroelectric dipoles and surface charges with slow relaxation dynamics in an external field lead to the emergence of a broad range of paraelectric-like, antiferroelectric-like ionic, and ferroelectric-like ferroionic states. The crossover between these states can be controlled not only by the static characteristics of the surface charges, but also by their relaxation dynamics in the applied field. Obtained results are not only promising for advanced applications of ferroelectric nanoparticles in nanoelectronics and optoelectronics, they also offer strategies for experimental verification.

36 MATERIALS SCIENCE↗

Self-Organization and Nitrogen Incorporation in Diamond-Like Carbon Microstructures Synthesized by Nonthermal Plasma

Nonthermal plasma activation of light alkanes is an encouraging decarbonization strategy to produce chemicals or fuels from abundant and/or flared carbon sources. However, prolific carbon growth on both the catalyst and electrode has limited its practicality, requiring additional knowledge of the carbon structure and growth mechanism before breakthroughs are realized. Furthermore, visual evidence is provided for nonuniform diamond-like carbon (DLC) microstructures that materialize in a coaxial dielectric barrier discharge (DBD) reactor flowing ethane and He at 278 K. Through a connection to known behaviors of DBD microdischarge patterns, the microstructure spacing was controlled by altering the applied voltage (ΔV) of the plasma or the burning voltage (U b ). Additionally, carbon valorization through nitrogen incorporation from N 2 was explored as an orthogonal solution to carbon mitigation, with N/C values >0.25 achieved and both sp 2 and sp 3 C–N bonding observed in the microstructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Piezoelectric domain walls in van der Waals antiferroelectric CuInP2Se6

Polar van der Waals chalcogenophosphates exhibit unique properties, such as negative electrostriction and multi-well ferrielectricity, and enable combining dielectric and 2D electronic materials. Using low temperature piezoresponse force microscopy, we revealed coexistence of piezoelectric and non-piezoelectric phases in CuInP2Se6, forming unusual domain walls with enhanced piezoelectric response. From systematic imaging experiments we have inferred the formation of a partially polarized antiferroelectric state, with inclusions of structurally distinct ferrielectric domains enclosed by the corresponding phase boundaries. The assignment is strongly supported by optical spectroscopies and density-functional-theory calculations. Enhanced piezoresponse at the ferrielectric/antiferroelectric phase boundary and the ability to manipulate this entity with electric field on the nanoscale expand the existing phenomenology of functional domain walls. At the same time, phase-coexistence in chalcogenophosphates may lead to rational strategies for incorporation of ferroic functionality into van der Waals heterostructures, with stronger resilience toward detrimental size-effects.

36 MATERIALS SCIENCE↗

Photoinduced Electron-Transfer Distance Is Controlled by the Driving Force in Solid-State Organic Donor-Acceptor Systems

Understanding how short-range electron transfer generates photocurrent in organic solar cells and what photochemical driving force is needed to maximize efficiencies has been an immensely difficult problem. Here we show how these questions are intertwined: the driving force controls the average charge-transfer distance, skipping the shortest-range states in the optimal case. Using photoinduced absorption-detected magnetic resonance, we measure average charge-separation distances in dilute donor–acceptor blends as a function of driving force, and compare these with free charge yields measured by time-resolved microwave conductivity. We find that the largest driving forces show the shortest charge-separation distances, explaining their suppressed free-carrier generation. These results support a long-range electron-transfer model, wherein the driving force controls the initial delocalization of the electron–hole pair. The minimum driving force required for efficient charge separation (and minimal voltage losses) is ultimately set by the dielectric constant of the material.

14 SOLAR ENERGY↗

Strongly temperature dependent ferroelectric switching in AlN, Al 1-x Sc x N, and Al 1-x B x N thin films

This manuscript reports the temperature dependence of ferroelectric switching in Al 0.84 Sc 0.16 N, Al 0.93 B 0.07 N, and AlN thin films. Polarization reversal is demonstrated in all compositions and is strongly temperature dependent. Between room temperature and 300 °C, the coercive field drops by almost 50% in all samples, while there was very small temperature dependence of the remanent polarization value. Furthermore, over this same temperature range, the relative permittivity increased between 5% and 10%. Polarization reversal was confirmed by piezoelectric coefficient analysis and chemical etching. Applying intrinsic/homogeneous switching models produces nonphysical fits, while models based on thermal activation suggest that switching is regulated by a distribution of pinning sites or nucleation barriers with an average activation energy near 28 meV.

36 MATERIALS SCIENCE↗