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At least 1,549 records · Page 86

Study of charge transport properties in a ZnO/CdS/Cu(In,Ga)Se 2 solar cell via admittance spectroscopy

The authors investigate the charge carrier transport properties in a thin-film heterojunction Cu(In,Ga)Se 2 (CIGS) solar cell device via coordinated capacitance-voltage and admittance spectroscopic measurements. The CIGS absorber width was measured using temperature dependent depletion width in the freeze-out regime and its acceptor density extracted from conventional capacitance-voltage analysis in the non-freeze-out regime. The bias-dependent modified dielectric relaxation in the Cu(In,Ga)Se 2 solar cell was exploited to extract the absorber's resistivity, hole mobility, and their temperature dependency, all by admittance spectroscopy. In the temperature range of 133-300 K, the extracted hole mobility in the CIGS device increases from 7.55 x 10 -3 to 4.08 cm 2 /Vs with temperature. The temperature dependent resistivity and mobility show Arrhenius behavior with an activation energy ~120 meV. The thermally activated behavior of mobility is related to the potential fluctuation encountered by the holes during their transport, which enables admittance spectroscopy to directly measure the potential fluctuation in the CIGS polycrystalline material.

14 SOLAR ENERGY↗

Wafer-scale high-k SrTiO 3 dielectrics with rational barrier-layer design for low leakage and high charge density

High-k oxides such as SrTiO 3 promise large capacitance, but their dielectric response is often limited by leakage currents due to reduced bandgaps. We show that introducing a thin barrier layer beneath SrTiO 3 is a simple and effective way to suppress leakage and increase charge density. Using hybrid molecular beam epitaxy, we grew uniform SrTiO 3 films on Nb:SrTiO 3 , CaSnO 3 /Nb:SrTiO 3 , and 2-in. SiO 2 /p-Si stacks to directly compare how different barrier layers influence device behavior. Both CaSnO 3 and SiO 2 reduce leakage, but the ultra-wide-bandgap SiO 2 layer enables much higher operating voltages, yielding charge densities exceeding 5 × 10 13 cm −2 at room temperature—more than a fivefold enhancement compared to devices without a barrier layer. This improvement comes with a predictable trade-off: the lower dielectric constant of SiO 2 reduces overall capacitance, making its thickness an important design parameter. Together, these results demonstrate that rational barrier-layer engineering—including wafer-scale integration on Si—provides a clear pathway to achieving higher charge densities in SrTiO 3 -based dielectric devices.

36 MATERIALS SCIENCE↗

Subwavelength resonant nanostructured films for sensing

We present a novel subwavelength nanostructure architecture that may be utilized for optical standoff sensing applications. The subwavelength structures are fabricated via a combination of nanoimprint lithography and metal sputtering to create metallic nanostructured films encased within a transparent media. The structures are based on the open ring resonator (ORR) architecture and have their analog in resonant LC circuits, which display a resonance frequency that is inversely proportional to the square root of the product of the inductance and capacitance. Therefore, any perturbation of the nanostructured films due to chemical or environmental effects can alter the inductive or capacitive behavior of the subwavelength features, which can shift the resonant frequency and provide an indication of the external stimulus. This shift in resonance can be interrogated remotely either actively using either laser illumination or passively using hyperspectral or multispectral sensing. These structures may be designed to be either anisotropic or isotropic, which can also provide polarization-sensitive interrogation. Due to the nanometer-scale of the structures, they can be tailored to be optically responsive in the visible or near infrared spectrum with a highly reflective resonant peak that is dependent solely on structural dimensions and material characteristics. We present experimental measurements of the optical response of these structures as a function of wavelength, polarization, and incident angle demonstrating the resonant effect in the near infrared region. Numerical modeling data showing the effect of different fabrication parameters such as structure parameters are also discussed.

Environmental Molecular Sciences Laboratory↗

Optically resonant subwavelength films for tamper-indicating tags and seals

We present the design, modeling and performance of a proof-of-concept tamper indicating approach that exploits newly-developed subwavelength-patterned films. These films have a nanostructure-dependent resonant optical reflection that is wavelength, angle, and polarization dependent. As such, they can be tailored to fabricate overlay transparent films for tamper indication and authentication of sensitive or controlled materials not possible with currently-known technologies. An additional advantage is that the unique optical signature is dictated by the geometry and fabrication process of the nanostructures in the film, rather than on the material used. The essential structure unit in the subwavelength resonant coating is a nanoscale Open-Ring Resonator (ORR). This building block is fabricated by coating a dielectric nanoscale template with metal to form a hemispherical shell-like structure. This curved metallic shell structure has a cross-section with an intrinsic capacitance and inductance and is thus the optical equivalent to the well-known “LC” circuit where the capacitance and inductance are determined by the nanoshell dimensions. For structures with sub 100 nm scale, this resonance occurs in the visible electromagnetic spectrum, and in the IR for larger shells. Tampering of the film would be visible though misalignment of the angular dependence of the features in the film. It is additionally possible to add in intrinsic oxidation and strain sensitive matrix materials to further complicate tamper repair and counterfeiting. Cursory standoff readout would be relatively simple using a combination of a near-infrared (or visible) LED flashlight and polarizer or passively using room lighting illumination and a dispersive detector.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Experimental determination of the PTW 60019 microDiamond dosimeter active area and volume

Purpose: Small field output correction factors have been studied by several research groups for the PTW 60019 microDiamond (MD) dosimeter, by comparing the response of such a device with both reference dosimeters and Monte Carlo simulations. A general good agreement is observed for field sizes down to about 1 cm. However, evident inconsistencies can be noticed when comparing some experimental results and Monte Carlo simulations obtained for smaller irradiation fields. This issue was tentatively attributed by some authors to unintentional large variations of the MD active surface area. The aim of the present study is a nondestructive experimental determination of the MD active surface area and active volume. Methods: Ten MD dosimeters, one MD prototype, and three synthetic diamond samples were investigated in the present work. 2D maps of the MD response were recorded under scanned soft x-ray microbeam irradiation, leading to an experimental determination of the device active surface area. Profiles of the device responses were measured as well. In order to evaluate the MD active volume, the thickness of the diamond sensing layer was independently evaluated by capacitance measurements and alpha particle detection experiments. The MD sensitivity, measured at the PTW calibration laboratory, was also used to calculate the device active volume thickness. Results: An average active surface area diameter of (2.19 ± 0.02) mm was evaluated by 2D maps and response profiles of all the MDs. Average active volume thicknesses of (1.01 ± 0.13) μm and (0.97 ± 0.14) μm were derived by capacitance and sensitivity measurements, respectively. The obtained results are well in agreement with the nominal values reported in the manufacturer dosimeter specifications. A homogeneous response was observed over the whole device active area. Besides the one from the device active volume, no contributions from other components of the housing nor from encapsulation materials were observed in the 2D response maps. Conclusions: The obtained results demonstrate the high reproducibility of the MD fabrication process. The observed discrepancies among the output correction factors reported by several authors for MD response in very small fields are very unlikely to be ascribed to unintentional variations of the device active surface area and volume. It is the opinion of the authors that the role of the volume averaging as well as of other perturbation effects should be separately investigated instead, both experimentally and by Monte Carlo simulations, in order to better clarify the behaviour of the MD response in very small fields.

60 APPLIED LIFE SCIENCES↗

Diffusion current in a system of coupled Josephson junctions

The role of a diffusion current in the phase dynamics of a system of coupled Josephson junctions (JJs) has been analyzed. It is shown that, by studying the temporal dependences of the superconducting, quasi-particle, diffusion, and displacement currents and the dependences of average values of these currents on the total current, it is possible to explain the main features of the current-voltage characteristic (CVC) of the system. The effect of a diffusion current on the character of CVC branching in the vicinity of a critical current and in the region of hysteresis, as well as on the part of CVC branch corresponding to a parametric resonance in the system is demonstrated. A clear interpretation of the differences in the character of CVC branching in a model of capacitively coupled JJs (CCJJ model) and a model of capacitive coupling with diffusion current (CCJJ+DC model) is proposed. It is shown that a decrease in the diffusion current in a JJ leads to the switching of this junction to an oscillating state. The results of model calculations are qualitatively consistent with the experimental data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electrically active centers formed in silicon during the high-temperature diffusion of boron and aluminum

The parameters of electrically active centers formed during the high-temperature diffusion of boron and aluminum into silicon in various media are studied by the Hall method and capacitance spectroscopy. It is found that the variation in the resistivity of the n base of the structures with p-n junctions fabricated in the study is controlled by the formation of three donor levels Q1, E4, and Q3 with the energies E{sub c} - 0.31, E{sub c} - 0.27, and E{sub c} - 0.16 eV. Diffusion in a chlorine-containing atmosphere introduces only a single level E4, but its concentration is 2.5 times lower, compared with diffusion in air. The values of the ionization energy of the Q3 level, measured under equilibrium (Hall effect) and nonequilibrium (capacitance spectroscopy) conditions, almost coincide. The deepest level E1 with an energy of E{sub c} - 0.54 eV, formed upon diffusion in both media, has no effect on the resistivity in the n base of the structures.

36 MATERIALS SCIENCE↗

Hopping conductivity and dielectric relaxation in Schottky barriers on GaN

A study of the current and capacitance dependences on the forward voltage in Au/n-GaN Schottky diodes, the sub-band optical absorption spectra, and the defect photoluminescence in n-GaN bulk crystals and thin layers is reported. It is shown that defect-assisted tunneling is the dominant transport mechanism for forward-biased Schottky contacts on n-GaN. The dependences of the current and capacitance on forward bias reflect the energy spectrum of defects in the band gap of n-GaN: the rise in the density of deep states responsible for yellow photoluminescence in GaN with increasing energy and the steep exponential tail of states with an Urbach energy of E{sub U} = 50 meV near the conduction-band edge. A decrease in the frequency of electron hops near the Au/n-GaN interface results in a wide distribution of local dielectric relaxation times and in a dramatic transformation of the electric-field distribution in the space-charge region under forward biases.

36 MATERIALS SCIENCE↗

Electrical properties and the determination of interface state density from I–V, C–f and G–f measurements in Ir/Ru/n-InGaN Schottky barrier diode

The electrical properties of the Ir/Ru Schottky contacts on n-InGaN have been investigated by current-voltage (I–V), capacitance-voltage (C–V), capacitance-frequency (C–f) and conductance-frequency (G–f) measurements. The obtained mean barrier height and ideality factor from I–V are 0.61 eV and 1.89. The built-in potential, doping concentration and barrier height values are also estimated from the C–V measurements and the corresponding values are 0.62 V, 1.20 × 1017 cm{sup –3} and 0.79 eV, respectively. The interface state density (N{sub SS}) obtained from forward bias I–V characteristics by considering the series resistance (R{sub S}) values are lower without considering the series resistance (R{sub S}). Furthermore, the interface state density (N{sub SS}) and relaxation time (τ) are also calculated from the experimental C–f and G–f measurements. The N{sub SS} values obtained from the I–V characteristics are almost three orders higher than the N{sub SS} values obtained from the C–f and G–f measurements. The experimental results depict that N{sub SS} and τ are decreased with bias voltage. The frequency dependence of the series resistance (R{sub S}) is attributed to the particular distribution density of interface states.

36 MATERIALS SCIENCE↗

First demonstration of 30 eVee ionization energy resolution with RICOCHET germanium cryogenic bolometers

The future RICOCHET experiment aims to search for new physics in the electroweak sector by measuring the Coherent Elastic Neutrino-Nucleus Scattering process from reactor antineutrinos with high precision down to the sub-100 eV nuclear recoil energy range. While the RICOCHET collaboration is currently building the experimental setup at the reactor site, it is also finalizing the cryogenic detector arrays that will be integrated into the cryostat at the Institut Laue Langevin in early 2024. In this paper, we report on recent progress from the Ge cryogenic detector technology, called the CryoCube. More specifically, we present the first demonstration of a 30 eVee (electron equivalent) baseline ionization resolution (RMS) achieved with an early design of the detector assembly and its dedicated High Electron Mobility Transistor (HEMT) based front-end electronics with a total input capacitance of about 40 pF. This represents an order of magnitude improvement over the best ionization resolutions obtained on similar phonon-and-ionization germanium cryogenic detectors from the EDELWEISS and SuperCDMS dark matter experiments, and a factor of three improvement compared to the first fully-cryogenic HEMT-based preamplifier coupled to a CDMS-II germanium detector with a total input capacitance of 250 pF. Additionally, we discuss the implications of these results in the context of the future RICOCHET experiment and its expected background mitigation performance.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Online Learning for Commercial Buildings

There has been an increased interest in designing optimization based techniques for the control of building heating, ventilation, and air-conditioning (HVAC) systems for either improving the energy efficiency of buildings or providing ancillary services to the electric grid. The performance of such prediction-based control techniques heavily rely on the model of a building’s thermal dynamics. However, the development of high fidelity building thermal dynamic models is challenging given the presence of large uncertainties that affect thermal loads in buildings such as building envelope performance, thermal mass, internal heat gains as well as occupants' behavior. In this paper, we propose a method to identify both a resistive-capacitive parametric model, and non -parametric load uncertainties using measured input-output data. The parametric model is obtained using semi-parametric regression, whereas the non-parametric part is based on Random Forest, where regression trees are used to derive the dependency of non-parametric terms on both building operation parameters and ambient temperature. The effectiveness of the method is evaluated using experimental data collected from an office building at the Pacific Northwest National Laboratory (PNNL) campus. The proposed methodology was observed to provide improved accuracy over appropriate baseline strategies, when predicting indoor air temperatures.

Dong, Jin↗

A Unidirectional Two-Compartment Neuron Circuit with On-chip STDP learning

Most neuromorphic chips implement the single-compartment point neuron model where synapse circuits connect directly to a leaky integrate and fire (LIF) soma circuit. However, when using a biologically plausible soma circuit (e.g., Hodgkin-Huxley neuron model), an interface circuitry, such as a current conveyor circuit, is needed to transmit synaptic current to the soma circuit. This is especially true for ultra-low power neuron circuits, where membrane capacitance is on the order of 20 fF. This need for an interface circuit arises because the parasitic capacitance and leakage current caused by fabrication mismatch and second-order effects of the output transistors in the synapse circuits can disturb the spiking dynamics of the soma circuit if connected without an interface. Using an interface circuit to isolate the soma’s membrane capacitor from synapses resolves this issue. We propose to use a unidirectional resistor (a transconductance circuit) to connect the synapse and soma circuits instead of conventional current conveyor circuits. Using a biologically plausible spike pattern detection model, we show that the on-chip spike-timing-dependent plasticity (STDP) learning performance of the proposed unidirectional two-compartment neuron circuit is similar to a single-compartment circuit (with a current conveyor as an interface) and additionally, it is more power-efficient and biologically plausible. The chip is fabricated in the Taiwan Semiconductor Manufacturing Company (TSMC) 250 nm technology node and comprises a single neuron circuit.

Gautam, Ashish [ORNL]↗

The Influence of Cr-Additives on the Polarization Resistance of Praseodymium-Doped Ceria Cathodes for Solid Oxide Fuel Cells

While Cr poisoning of the oxygen reduction reaction (ORR) at SOFC cathodes is widely agreed to involve deactivation of oxygen exchange sites, the degradation mechanism remains ambiguous. Here, we selected an alternative cathode material Pr 0.1 Ce 0.9 O 2− δ , free of Sr segregation, to systematically investigate the effect of Cr-induced degradation in ORR. We expand on our previous studies in which the acidity/basicity of binary additives was found to be a strong indicator of the rate of oxygen surface exchange, by electrochemically investigating the ORR activity of the PCO cathode by impedance spectroscopy. Serial infiltration with acidic Cr-based oxides was found to degrade ORR activity as reflected in a 20-fold increase in area specific resistance (ASR) without corresponding changes in activation energy, with the opposite trend obtained with Ca-based oxides. Detected changes in total capacitance, attributed to changes in surface capacitance, also suggest depressed/enhanced PCO surface redox behavior with Cr/Ca-based infiltrants. Taken together, these results point to a more universal source of ORR poisoning/activation, based on acidity/basicity, rather than physical blocking of active sites. With this improved understanding, one can expect progress to be made in the coming years in optimizing means for protecting catalytic surfaces from degradation and/or improving their performance.

25 ENERGY STORAGE↗

Pseudocapacitive Charge Storage in Electrochromic Transition-Metal Oxide Thin Films

Electrochromic pseudocapacitive transition-metal oxide materials, such as tungsten oxide, which combine fast response, high energy density, and optical effects, can play a significant role as energy storage materials. Here we investigate the electrochemical kinetics of thin films of tungsten oxide, which turn transparent to sky-blue color in the lithiated state due to the reduction of W 6+ to W 5+ . In this study, we investigated the charge density, charge transfer, ion diffusion, and interfacial behavior upon Li + insertion/de-insertion in WO 3 . The electrochromic thin film's pseudocapacitive and electrical double layer mechanism was differentiated based on the power-law. Faradaic diffusion-controlled process dominates over the surface capacitive behavior at scan rates below 40 mV s –1 . These films exhibit an areal charge density of around 100 mC cm –2 and a capacitance of 80 mF cm –2 , superior to most comparable electrochromic materials and supercapacitors. This work combines electrochromics and energy storage properties and provides a fundamental understanding of pseudocapacitive and electrochromic mechanisms in WO 3 .

25 ENERGY STORAGE↗

Flowable conducting particle networks in redox-active electrolytes for grid energy storage

This paper reports a new hybrid approach toward achieving high volumetric energy and power densities in an electrochemical flow capacitor for grid energy storage. The electrochemical flow capacitor suffers from high self-discharge and low energy density because charge storage is limited to the available surface area (electric double layer charge storage). Here, we examine two carbon materials as conducting particles in a flow battery electrolyte containing the VO 2+ /VO 2 + redox couple. Highly porous activated carbon spheres (CSs) and multi-walled carbon nanotubes (MWCNTs) are investigated as conducting particle networks that facilitate both faradaic and electric double layer charge storage. Charge storage contributions (electric double layer and faradaic) are distinguished for flow-electrodes composed of MWCNTs and activated CSs. A MWCNT flow-electrode based in a redox-active electrolyte containing the VO 2+ /VO 2 + redox couple demonstrates 18% less self-discharge, 10 X more energy density, and 20 X greater power densities (at 20 mV s -1 ) than one based on a non-redox active electrolyte. Additionally, a MWCNT redox-active flow electrode demonstrates 80% capacitance retention, and >95% coulombic efficiency over 100 cycles, indicating the feasibility of utilizing conducting networks with redox chemistries for grid energy storage.

25 ENERGY STORAGE↗

Cation Molecular Structure Affects Mobility and Transport of Electrolytes in Porous Carbons

We examined the electrosorption and ion dynamics of imidazolium-based room temperature ionic liquids (RTILs) having short (3-carbon, C3mim + ) and long (12-carbon, C12mim + ) cations, that is, 1-propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (C3mimTFSI) and 1-dodecyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (C12mimTFSI), confined in ordered mesoporous carbon (OMC) and analyzed the influence of the cation alkyl chain length on the ion dynamics and the capacitive behavior using electrochemical measurements together with quasi-elastic neutron scattering (QENS) observations and classical density functional theory (cDFT) computations. Electrochemical tests highlighted the significant influence of specific applied potentials on accumulated charge storage densities and on the limits of saturation of larger electrolytes in the pores. Computational analyses corroborated these findings and predicted a 16% increase in the capacitance of the smaller-cation electrolyte under high applied potentials. However, QENS experiments revealed a behavior of decoupling of alkyl chain dynamics from the ring in electrolytes with larger ions. cDFT calculations identified density spikes for C12mim + away from the pore walls to further corroborate this unique behavior. Here, our insights into chain length-dependent dynamics and electrosorption in complex electrolyte-electrode systems deepen fundamental understanding of confined RTIL electrolyte behavior in the porous carbon electrodes.

25 ENERGY STORAGE↗

Understanding Artifacts in Impedance Spectroscopy

Four-terminal measurements of impedance spectra have long been troubled by the presence of high frequency artifacts that typically indicate unphysically large inductive behavior. In this paper, we follow up on the observation of Fleig et al., that voltage and current are necessarily measured in different locations of the potentiostat circuit, and that, typically, the electrometer input is a virtual ground. In this case, the capacitance of coaxial cables that connect sample electrodes to the potentiostat provides a high frequency conduction path to ground, so that some of the current that passes through the sample bypasses the electrometer. In four-electrode measurements, this mechanism produces the observed inductive artifacts. We examine a variety of simulated samples, with calculations compared to measurements of relevant circuits, to quantitatively investigate the nature of the artifacts. Model results agree with measurements when the leakage capacitances are properly included in the circuit analyses. With understanding of the origin of the inductive artifacts, the four-electrode method can be effectively utilized, enabling a combination of two-, three- and four-electrode measurements to be used to best advantage. Finally, using this combination of electrode configurations, temperature dependent measurements of SrTiO 3 , Y 2 O 3 -stabilized ZrO 2 , and In 2 O 3 films deposited on YSZ substrates are presented.

36 MATERIALS SCIENCE↗

Coupling Schemes in Terahertz Planar Metamaterials

We present a review of the different coupling schemes in a planar array of terahertz metamaterials. The gap-to-gap near-field capacitive coupling between split-ring resonators in a unit cell leads to either blue shift or red shift of the fundamental inductive-capacitive ( LC ) resonance, depending on the position of the split gap. The inductive coupling is enhanced by decreasing the inter resonator distance resulting in strong blue shifts of the LC resonance. We observe the LC resonance tuning only when the split-ring resonators are in close proximity of each other; otherwise, they appear to be uncoupled. Conversely, the higher-order resonances are sensitive to the smallest change in the inter particle distance or split-ring resonator orientation and undergo tremendous resonance line reshaping giving rise to a sharp subradiant resonance mode which produces hot spots useful for sensing applications. Most of the coupling schemes in a metamaterial are based on a near-field effect, though there also exists a mechanism to couple the resonators through the excitation of lowest-order lattice mode which facilitates the long-range radiative or diffractive coupling in the split-ring resonator plane leading to resonance line narrowing of the fundamental as well as the higher order resonance modes.

Roy Chowdhury, Dibakar↗