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DOE OSTI2024

Size Effect of Negative Capacitance State and Subthreshold Swing in Van der Waals Ferrielectric Field–Effect Transistors

Analytical calculations corroborated by the finite element modeling show that thin films of Van der Waals ferrielectrics covered by a 2D-semiconductor are promising candidates for the controllable reduction of the dielectric layer capacitance due to the negative capacitance (NC) effect emerging in the thin films. The NC state is conditioned by energy-degenerated poly-domain states of the ferrielectric polarization induced in the films under incomplete screening conditions in the presence of a dielectric layer. Calculations performed for the FET-type heterostructure “ferrielectric CuInP 2 S 6 film—2D-MoS 2 single-layer—SiO 2 dielectric layer” reveal the pronounced size effect of the multilayer capacitance. Derived analytical expressions for the electric polarization and multilayer capacitance allow to predict the thickness range of the dielectric layer and ferrielectric film for which the NC effect is the most pronounced in various Van der Waals ferrielectrics, and the corresponding subthreshold swing becomes much less than the Boltzmann's limit. Obtained results can be useful for the size and temperature control of the NC effect in the steep-slope ferrielectric FETs.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Reducing the Susceptibility of Lumped-Element KIDs to Two-Level System Effects

Arrays of lumped-element kinetic inductance detectors (LEKIDs) optically coupled through an antenna-coupled transmission line are a promising candidate for future cosmic microwave background experiments. However, the dielectric materials used for the microstrip architecture are known to degrade the performance of superconducting resonators. In this paper, we investigate the feasibility of microstrip coupling to a LEKID, focusing on a systematic study of the effect of depositing amorphous silicon nitride on a LEKID. The discrete and spatially separated inductive and capacitive regions of the LEKID allow us to vary the degree of dielectric coverage and determine the limitations of the microstrip coupling architecture. We show that by careful removal of dielectric from regions of high electric field in the capacitor, there is minimal degradation in dielectric loss tangent of a partially covered lumped-element resonator. We present the effects on the resonant frequency and noise power spectral density and, using the dark responsivity, provide an estimate for the resulting detector sensitivity.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Effects of Asymmetric Molecular Architecture on Chain Stretching and Dynamics in Miktoarm Star Copolymers

We use broad-band dielectric spectroscopy (BDS) and small-angle X-ray scattering (SAXS) to investigate the impact of architectural asymmetry in the miktoarm star copolymer on the dielectric polymer relaxations. The miktoarm copolymers studied contain one or two polystyrene (PS) chains of constant molecular weight and two identical poly(cis-1,4-isoprene) (PI) chains with varied molecular weights. Using the chains in the PI block as dielectric probes, we find that the architecturally asymmetric miktoarm star copolymer systems (PSPI 2 ) feature distributions in chain relaxation times and dielectric relaxation strengths that are not dependent on molecular weight or morphology, in stark contrast to the effects of morphological confinement observed for symmetric diblock systems (PS-b-PI or PS 2 PI 2 ). Along with evidence from the SAXS measurements regarding phase separation, these results are attributed to influences from chain stretching within the framework of the Gaussian chain model for block copolymer systems. As such, the molecular architecture in block copolymers happens to be a versatile handle to control polymer chain dynamics and, ultimately, the macroscopic physicochemical properties in architecturally complex polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Concentration-dependent ion correlations impact the electrochemical behavior of calcium battery electrolytes.

Ion interactions strongly determine the solvation environments of multivalent electrolytes even at concentrations below that required for practical battery-based energy storage. This statement is particularly true of electrolytes utilizing ethereal solvents due to their low dielectric constants. These solvents are among the most commonly used for multivalent batteries based on reactive metals (Mg, Ca) due to their reductive stability. Recent developments in multivalent electrolyte design have produced a variety of new salts for Mg2+ and Ca2+ that test the limits of weak coordination strength and oxidative stability. Such electrolytes have great potential for enabling full-cell cycling of batteries based on these working ions. However, the ion interactions in these electrolytes exhibit significant and non-intuitive concentration relationships. In this work, we investigate a promising exemplar, calcium tetrakis(hexafluoroisopropoxy)borate (Ca(BHFIP)(2)), in the ethereal solvents 1,2-dimethoxyethane (DME) and tetrahydrofuran (THF) across a concentration range of several orders of magnitude. Surprisingly, we find that effective salt dissociation is lower at relatively dilute concentrations (e.g. 0.01 M) than at higher concentrations (e.g. 0.2 M). Combined experimental and computational dielectric and X-ray spectroscopic analyses of the changes occurring in the Ca2+ solvation environment across these concentration regimes reveals a progressive transition from well-defined solvent-separated ion pairs to de-correlated free ions. This transition in ion correlation results in improvements in both conductivity and calcium cycling stability with increased salt concentration. Comparison with previous findings involving more strongly associating salts highlights the generality of this phenomenon, leading to important insight into controlling ion interactions in ether-based multivalent battery electrolytes.

Hahn, Nathan T.↗

DOE OSTI2024

Resilience of the Aurivillius structure upon La and Cr doping in a Bi 5 Ti 3 FeO 15 multiferroic

Here, combining the experimental techniques of high-resolution X-ray diffraction, magnetometry, specific heat measurement, and X-ray photoelectron, Raman and dielectric spectroscopy techniques, we have studied the influence of La and Cr doping on the crystal structure and magnetism of the room temperature Aurivillius multiferroic Bi 5 Ti 3 FeO 15 by investigating the physical properties of (Bi 4 La)Ti 3 FeO 15 and Bi 5 Ti 3 (Fe 0.5 Cr 0.5 )O 15 . The parent (Bi 5 Ti 3 FeO 15 ) and the doped ((Bi 4 La)Ti 3 FeO 15 and Bi 5 Ti 3 (Fe 0.5 Cr 0.5 )O 15 ) compounds crystallize in the A2 1 am space group, which is confirmed through our analysis of high-resolution synchrotron X-ray diffraction data obtained on phase-pure polycrystalline powders. We determined the oxidation states of the metal atoms in the studied compounds as Fe 3+ , Ti 4+ , Cr 3+ , and La 3+ through the analysis of X-ray photoelectron spectroscopy data. The magnetic susceptibilities of the three compounds are marked by the absence of a long-range ordered ground state, but dominated by superparamagnetic clusters with dominant antiferromagnetic interactions. This signature of short-range magnetism is also seen in specific heat as a low temperature enhancement which is suppressed upon the application of external magnetic fields up to 8 T. Our dielectric spectroscopy experiments showed that the three studied compounds display similar features in the dielectric constant measured as a function of frequency. However, upon doping La at the Bi site, the width of the ferroelectric hysteresis loop increases for (Bi 4 La)Ti 3 FeO 15 compared to that of the parent compound Bi 5 Ti 3 FeO 15 , and with Cr doping, Bi 5 Ti 3 (Fe 0.5 Cr 0.5 )O 15 becomes a leaky dielectric. The resilience of the Aurivillius crystal structure towards doping of La at the Bi site and Cr at the Fe site is clearly seen in the bulk properties of magnetic susceptibility, specific heat and the average crystal structure. The relevance of changes in the local structure is evident from our Raman spectroscopy and X-ray pair distribution function studies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

NaCl aggregation in water at elevated temperatures and pressures: Comparison of classical force fields

The properties of water vary dramatically with temperature and density. This can be exploited to control its effectiveness as a solvent. Thus, supercritical water is of keen interest as solvent in many extraction processes. The low solubility of salts in lower density supercritical water has even been suggested as a means of desalination. The high temperatures and pressures required to reach supercritical conditions can present experimental challenges during collection of required physical property and phase equilibria data, especially in salt-containing systems. Molecular simulations have the potential to be a valuable tool for examining the behavior of solvated ions at these high temperatures and pressures. However, the accuracy of classical force fields under these conditions is unclear. We have, therefore, undertaken a parametric study of NaCl in water, comparing several salt and water models at 200 bar–600 bar and 450 K–750 K for a range of salt concentrations. We report a comparison of structural properties including ion aggregation, hydrogen bonding, density, and static dielectric constants. All of the force fields qualitatively reproduce the trends in the liquid phase density. An increase in ion aggregation with decreasing density holds true for all of the force fields. The propensity to aggregate is primarily determined by the salt force field rather than the water force field. This coincides with a decrease in the water static dielectric constant and reduced charge screening. While a decrease in the static dielectric constant with increasing NaCl concentration is consistent across all model combinations, the salt force fields that exhibit more ionic aggregation yield a slightly smaller dielectric decrement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Surface ionization waves propagating over non-planar substrates: wavy surfaces, cut-pores and droplets

Atmospheric pressure plasmas intersecting with dielectric surfaces will often transition into surface ionization waves (SIWs). Several applications of these discharges are purposely configured to be SIWs. During propagation of an SIW over a dielectric surface, the plasma charges the surface while responding to changes in geometrical and electrical material properties. This is particularly important for non-planar surfaces where polarization of the dielectric results in local electric field enhancement. In this paper, we discuss results from computational investigations of negative and positive SIWs propagating over nonplanar dielectrics in three configurations—wavy surfaces, cuts through porous materials and water droplets on flat surfaces. Here we found that negative SIWs are particularly sensitive to the electric field enhancement that occurs at the crests of non-planar surfaces. The local increase in ionization rates by the electric field enhancement can result in the SIW detaching from the surface, which produces non-uniform plasma exposure of the surface. Positive SIWs tend to adhere to the surface to a greater degree. These trends indicate that treatment of pathogen containing droplets on surfaces may be best performed by positive SIWs. The same principles apply to the surfaces cut through pores. Buried pores with small openings to the SIW may be filled by plasma by either flow of plasma into the pore (large opening) or initiated by photoionization (small opening), depending on the size of the opening compared to the Debye length.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Probing phonon softening in ferroelectrics by scanning probe microwave spectroscopy

Microwave measurements have recently been successfully applied to measure ferroelectric materials on the nanoscale, including detection of polarization switching and ferroelectric domain walls. In this study we discuss the question of whether scanning probe microscopy operating at microwave frequency can identify the changes associated with the soft phonon dynamics in a ferroic. The analytical expressions for the electric potential, complex impedance, and dielectric losses are derived and analyzed, since these physical quantities are linked to experimentally measurable properties of the ferroic. As a ferroic we consider virtual or proper ferroelectric with an optic phonon mode that softens at a Curie point. We also consider a decay mechanism linked to the conductance of the ferroic, thus manifesting itself as the dielectric loss in the material. Our key finding is that the influence of the soft phonon dispersion on the surface potential distribution, complex impedance, and dielectric losses are evidently strong in the vicinity (~10–30 K) of the Curie temperature. Additionally, we quantified how the spatial distribution and frequency spectra of the complex impedance and the dielectric losses react on the dynamics of the soft phonons near the Curie point. These results set the stage for characterization of polar phase transitions with nanoscale microwave measurements, providing a complementary approach to well established electromechanical measurements for fundamental understanding of ferroelectric properties as well as their applications in telecommunication and computing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Giant Polarization in Nanodielectrics

The relative permittivity of a material is a scaling factor for capacitors and the devices based upon them; the larger the relative permittivity, the greater the degree of miniaturization, or potential for energy storage. Materials with a relative permittivity than that of silicon nitride (approximately 7) are referred to as high-dielectric constant materials. Values of about 100 are typical in titanium dioxide rutile. Values of about 10,000 are observed in barium titanate in the region of the ferroelectric transition, which while impressive, is not very useful due to the strong temperature dependence. The observation of a relative permittivity of over 100,000 in the calcium copper titanate material sparked considerable interest because it showed little temperature dependence between 100 and 600 K over most of the radio-frequency range. Further investigation revealed that this material appears to be naturally nanotextured and that the colossal permittivity was likely due to the surface and/or internal barrier layer capacitance effect, although the issue is not settled. Unfortunately, the dielectric losses in this class materials are relatively high. A new strategy to achieve high dielectric permittivity with low loss involves using localized lattice defect states through ambipolar co-doping; these intrinsic defect complexes give rise to strong dipoles that are responsible for a relative permittivity of 10,000 with exceptionally low dielectric losses over most of the radio frequency range and excellent thermal stability.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Design and fabrication of ion traps for low RF power dissipation

Large surface-electrode ion traps with multiple trapping regions and junctions are a natural approach to scaling trapped ion quantum computers, supporting the connectivity and ion counts necessary for complex quantum algorithms. However, a major hurdle in this scaling is on-chip power dissipation from the applied RF voltage, which increases at a rate between linear and cubic relative to trap size, depending on whether the losses are dielectric or Ohmic. Here, we present two versions of a trap with features designed to reduce both types of RF power dissipation. The first variant contains a raised RF electrode that increases the electrode–ground distance to reduce capacitance. Different DC voltage sources are demonstrated on this trap to show that technical noise before the filter remains the dominant source of voltage noise and therefore motional heating. The second variant additionally includes a method for removing dielectric from beneath the RF electrode to further reduce dielectric losses. These traps were demonstrated at room temperature with 40 Ca + ions. In conclusion, the similar heating rates and heating rate axial frequency dependencies between 2.4 and 3.0 MHz illustrate that this dielectric modification is not detrimental to trap performance.

Sterk, J. D. [Sandia National Laboratories (SNL-NM↗

DOE OSTI2022

Optical properties of Mo and amorphous MoOx, and application to antireflection coatings for metals

To form antireflection (AR) coatings to hide metal architecture in display technologies, we deposited thin films of metal Mo and oxide MoOx by sputtering targets of various compositions using pure Ar sputter gas. The optical constants [n,k] of these samples were measured by the direct numerical solution of reflectance and transmittance at each wavelength point measured. We find that 50 nm films are uniform in the growth direction, but for thicker 100 nm samples, evidence exists for nonuniform growth, where the top 20 nm appears to be metal rich. From these [n,k], negative Tauc bandgap energies show these oxides are semi-metals. We then identified the specific composition (x) that optimizes the AR response for a host of metals (Al, Cu, Ag, Au). Finally, two methods were used to understand why these MoOx materials function well as AR media, including (i) using phasor rays and (ii) developing a universal expression for the AR condition that applies to both dielectric and metal substrates. In (i), we find two characteristics for AR of metals: (a) its optical thickness should be roughly π3, not the π2 for dielectrics, since for MoOx, their [r^ij,t^ij] Fresnel phases differ from the usual [180°, 0°] of dielectrics; and (b) the medium incorporates a k-dominant strategy whose function is to absorb the energy that is reflected at the AR/metal interface. In (ii), the universal AR condition is found to be r^01+r^12z^=0. For dielectrics, this reduces to the well-known nAR=nairnsub condition. However, for metals, a concise analytic expression is lacking since this expression is highly nonlinear but is easily solved by numerical methods.

Tsu, David V. (ORCID:0000000295903418)↗

DOE OSTI2024

Active Aerodynamic Load Control for Wind Turbines

The goal of this project was to develop and demonstrate an advanced dielectric barrier discharge (DBD) plasma actuator technology. We set out to demonstrate the efficacy and impact of the new actuator technology as a key component of an active load control system for wind turbines. A DBD plasma actuator consists of a thin layer of dielectric material separating a pair of offset electrodes. One of those electrodes is embedded between the dielectric layer and a non-conductive substrate, while the other is exposed to air. When driven by an appropriate high voltage waveform, the device ionizes the air near the surface of the dielectric and adjacent to the exposed electrode. Collisions between the ions in the plasma and neutral air molecules result in a wall-jet – a region of induced air velocity that can be used to modify the flow around a lifting body. Use of the device near the trailing edge of a wind turbine blade, designed in such a way as to amplify the effects of the flow-modifying device, can result in large changes to the global forces experienced by the blade. Because of the fast response time of the device, it can allow the turbine to react in real time to changes in the wind associated with turbulence, wind shear, gusts, and the like, when paired with appropriate sensors and control algorithms. The goal of this project was to increase the capacity of the device to induce velocity on its surface at the levels required by large, utility-scale wind turbines. The first technical goal was to increase the induced velocity from the current industry-best of about 4 m/s to 10 m/s by modifying the electrical waveform used to drive the device and by introducing a semi-conductive surface coating to control electrostatic charge build-up on the surface. The second goal was to use the device to modify the lift on a representative airfoil in a wind tunnel, demonstrating a reduction in lift coefficient of 0.2 or better. The third goal was to produce an actuator-induced velocity of 20 m/s. Alongside our partners at the University of Texas at Dallas, we also applied modern, advanced design methods to optimize the impact of the technology on the design of wind turbines. We also had planned to install a segmented, active load control system on a test turbine to demonstrate the ability to reduce unsteady aerodynamic forces on the turbine associated with changes in the wind. The highest induced velocity achieved during this research was 11 m/s. However, practical design constraints limited the change in lift coefficient to about 0.12 for a representative airfoil in the wind tunnel at a Reynolds number of 400,000. The primary conclusion is that the plasma actuator control authority remains insufficient for practical purposes when extrapolated to Reynolds numbers over 1 million. The potential impact of the active lift control concept was evaluated through detailed simulations for three wind turbine sizes: a 3.4MW onshore turbine, a 10MW offshore turbine, and a 15MW offshore turbine. A feedback control system was designed for each turbine within two scenarios: one where the active lift control is used as a retrofit capability on the baseline design, and the other where the designers were permitted to “upscale” the turbines in order increase annual energy production. The levelized cost of energy was then evaluated for the range of turbine sizes and design configuration. It was found that the LCOE reduction associated with active lift control fell in the range of 0.7% to 7.2%, with the highest reduction associated with upscaling the 3.4MW turbine.

17 WIND ENERGY↗

DOE OSTI2024

Solution-Based Synthesis of Ultrathin Quasi-2D Amorphous Carbon for Nanoelectronics

The synthesis of ultrathin 2D amorphous dielectric film represents a major challenge due to the metastable nature of amorphous phases. We describe a scalable and solution-based strategy to prepare wafer-scale 2D amorphous carbon with thickness down to 1–2 atomic layers from coal-derived carbon quantum dots as precursors. The prepared atomically thin 2D amorphous carbon can be suspended over cavities as freestanding membranes with high modulus of 400±100 GPa and demonstrate robust dielectric properties with dielectric strength above 20 MV·cm-1 and leakage current density below 10-4 A·cm-2 through a scaled thickness of three-atomic layers. When implemented as ultrathin gate dielectrics in 2D transistors or ion-transport media in memristors, they enable exceptional device performance and spatiotemporal uniformity, resulting from their amorphous form, intrinsic ultrathinness, and 2D atomic structures.

Pham, Viet Hung [NETL Site Support Contractor, Nat↗

DOE OSTI2025

Investigating Low Loss Substrates for Improved Qubit Coherence Times

Superconducting qubits are sensitive to dielectric losses from substrates, making the identification, optimization, and preparation of low-loss materials essential for enhancing qubit coherence times. In this work, we utilize Nb superconducting radio-frequency (SRF) cavities as a high-precision measurement tool to study the dielectric loss tangent of substrates with parts-per-billion sensitivity. This technique enables temperature- and field-resolved measurements, providing deep insights into the behavior of candidate materials such as sapphire and silicon. We explore the impact of substrate preparation techniques, examining how surface treatments and cleaning protocols influence dielectric loss. These studies highlight both the microscopic origins of loss in these substrates and the critical role of preparation methods, helping to identify key materials and processes that minimize dielectric loss, crucial for improving qubit performance.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Electro-Thermo-Mechanical (ETM) Study on Submarine Dynamic Power Cables (SDPC) for Offshore Wind Transmission

Understanding the failure mechanisms of submarine dynamic power cables (SDPC) is critical for innovative design to meet the 2035 cost reduction target of U.S. DOE Floating Offshore Wind Shot. This is important because the current design suffers a significant failure rate in the field. This project conducted a systematic electro-thermo-mechanical (ETM) experimental study on the power cores extracted from a 15kV power cable with three cores of copper conductor, ethylene propylene rubber (EPR) insulation, and continuously corrugated welded aluminum armor (CCWA). An ETM testing system was developed by integrating a high voltage (HV) amplifier, two ceramic heaters, and a rod-plate transverse compression setup into a mechanical testing machine. Increasing temperature from room temperature (RT, 22 degree C) to 90 degree C resulted in the 67% decrease in the failure mechanical load as defined by the dielectric breakdown. Under creep mechanical loading, the dielectric breakdown time was decreased by 70% for a given mechanical load when the specimen temperature increased from RT to 90oC. The failure strain in both monotonic and creep mechanical loading modes was related to the maximum mechanical load applied. Although the dielectric breakdown occurred in the ETM test, the post-test measurement revealed an impressive recovery of electric resistance. The failure analysis on cross section of tested specimens indicated a sizable gap across insulation layer near the area between copper conductor and loading rod, which apparently resulted from online dielectric failure and offline elastic recovery of components including conductor and insulation layer.

17 WIND ENERGY↗

DOE OSTI2020

Disk-integrated Thermal Properties of Ceres Measured at Millimeter Wavelengths

We observed Ceres at three epochs in 2015 November and 2017 September and October with Atacama Large Millimeter/submillimeter Array (ALMA) 12 m array and in 2017 October with the ALMA Compact Array (ACA), all at ∼265 GHz continuum (wavelengths of ∼1.1 mm) to map the temperatures of Ceres over a full rotation at each epoch. We also used 2017 October ACA observations to search for HCN. The disk-averaged brightness temperature of Ceres is measured to be between 170 and 180 K during our 2017 observations. The rotational light curve of Ceres shows a double-peaked shape with an amplitude of about 4%. Our HCN search returns a negative result with an upper limit production rate of ∼2 × 10{sup 24} molecules s{sup −1}, assuming globally uniform production and a Haser model. A thermophysical model suggests that Ceres’s top layer has higher dielectric absorption than lunar-like materials at a wavelength of 1 mm. However, previous observations showed that the dielectric absorption of Ceres decreases toward longer wavelengths. Such distinct dielectric properties might be related to the hydrated phyllosilicate composition of Ceres and possibly abundant micrometer-sized grains on its surface. The thermal inertia of Ceres is constrained by our modeling as likely being between 40 and 160 thermal inertia units, much higher than previous measurements at infrared wavelengths. Modeling also suggests that Ceres’s light curve is likely dominated by spatial variations in its physical or compositional properties that cause changes in Ceres’s observed thermal properties and dielectric absorption as it rotates.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Giant polarization in nanodielectrics

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Electronic assembly with a direct current bus connection

A folded outer tab comprises a first outer dielectric layer and a second outer dielectric layer that contact or overlie an outer terminal, where the outer terminal is associated with a first polarity of the DC bus. A bent inner tab comprises a first inner dielectric layer and a second inner dielectric layer that contact or overlie an inner terminal, where the inner terminal is associated with a second polarity of the DC bus that is opposite the first polarity. The folded outer tab and the bent inner tab comprise electrically conductive faces, of opposite polarities, formed of exposed portions of the outer terminal and the inner terminal.

Schmit, Christopher J.↗