Development of solid-state avalanche amorphous selenium for medical imaging: Solid-state avalanche amorphous selenium sensor
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Scheuermann, James R.↗
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The flush-mounted rail Langmuir probe array designed for the Alcator C-Mod vertical target plate divertor
An array of flush-mounted and toroidally elongated Langmuir probes (henceforth called rail probes) have been specifically designed for the Alcator C-Mod’s vertical target plate divertor and operated over multiple campaigns. The “flush” geometry enables the tungsten electrodes to survive high heat flux conditions in which traditional “proud” tungsten electrodes suffer damage from melting. The toroidally elongated rail-like geometry reduces the influence of sheath expansion, which is an important effect to consider in the design and interpretation of flush-mounted Langmuir probes. The new rail probes successfully operated during C-Mod’s FY2015 and FY2016 experimental campaigns with no evidence of damage, despite being regularly subjected to heat flux densities parallel to the magnetic field exceeding ~1 GW m -2 for short periods of time. A comparison between rail and proud probe data indicates that sheath expansion effects were successfully mitigated by the rail design, extending the use of these Langmuir probes to incident magnetic field line angles as low as 0.5°.
47 OTHER INSTRUMENTATION↗
Microscale 2.5D Batteries
3D solid-state batteries use vertical topography to increase both energy and power density relative to batteries with planar geometry. Here we investigate, using finite element simulations, a battery that incorporates a 3D cathode consisting of a vertical array of microcolumns, and a planar 2D anode, which we call a 2.5D battery. By confining the 3D structure to the cathode we greatly simplify the battery fabrication process (i.e., 3D structure only needs to be introduced into one electrode) at the cost of introducing a non-uniform electrolyte thickness in which the anode-cathode distance varies significantly across different parts of the battery. We use simulations to show that a non-uniform electrolyte thickness results in inhomogeneous lithiation and subsequent underutilization of the cathode. The underutilization of the cathode can be avoided by using an electrolyte with sufficient ionic conductivity, which suggests that non-uniform electrolyte thickness can be tolerated in high ionic conductivity electrolytes but should be avoided in low ionic conductivity electrolytes.
25 ENERGY STORAGE↗
Characterizing Enzymatic Deposition for Microelectrode Neurotransmitter Detection
The enzyme immobilization process, one step in creating an enzymatic biosensor, was characterized and analyzed as a function of its physical properties. The neural glutamic biosensor is a flexible device, effectively minimizing trauma to the area of implantation. The Multielectrode Array (MEA) is composed primarily of a proprietary polymer which has been successfully implanted into human subjects in recent years. This polymer allows the device the pliability that other devices normally lack, though this poses some challenges to implantation. The electrodes are made of Platinum (Pt), and can range in number from eight to thirty two electrodes per device. These electrodes are electroplated with a semipermeable polymer layer to improve selectivity of the electrode to the neurotransmitter of interest, in this case glutamate. A signal is created from the interaction of glutamate in the brain with the glutamate oxidase (GluOx) which is immobilized on the surface of the electrode by using crosslinking chemistry in conjunction with glutaraldehyde and Bovine Serum Albumin (BSA). The glutamate is oxidized by glutamate oxidase, producing α-ketoglutarate and hydrogen peroxide (H 2 O 2 ) as a by-product. The production of H 2 O 2 is crucial for detection of the presence of the glutamate within the enzymatic coating, as it diffuses through the enzyme layer and oxidizes at the surface of the electrode. This oxidation is detectable by measurable change in the current using amperometry. Hence, the MEA allows for in vivo monitoring of neurotransmitter activity in real time. The sensitivity of the sensor to these neurotransmitters is dependent on the thickness of the layer, which is investigated in these experiments in order to optimize the efficacy of the device to detecting the substrate, once implanted.
59 BASIC BIOLOGICAL SCIENCES↗
The flush-mounted rail Langmuir probe array designed for the Alcator C-Mod vertical target plate divertor
An array of flush-mounted and toroidally elongated Langmuir probes (henceforth called rail probes) have been specifically designed for the Alcator C-Mod’s vertical target plate divertor and operated over multiple campaigns. The “flush” geometry enables the tungsten electrodes to survive high heat flux conditions in which traditional “proud” tungsten electrodes suffer damage from melting. The toroidally elongated rail-like geometry reduces the influence of sheath expansion, which is an important effect to consider in the design and interpretation of flush-mounted Langmuir probes. The new rail probes successfully operated during C-Mod’s FY2015 and FY2016 experimental campaigns with no evidence of damage, despite being regularly subjected to heat flux densities parallel to the magnetic field exceeding ∼1 GW per square meter for short periods of time. A comparison between rail and proud probe data indicates that sheath expansion effects were successfully mitigated by the rail design, extending the use of these Langmuir probes to incident magnetic field line angles as low as 0.5 degree.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Autonomous light management system for a window and method of controlling light transmission
An autonomous light management system for a window includes an electrochromic film stack comprising an electrochromic layer on a first transparent electrode, an ion storage layer on a second transparent electrode, and an electrolyte sandwiched between the ion storage and electrochromic layers. The electrochromic film stack exhibits a transmissive state or an absorptive state depending on charging or discharging of the electrochromic layer. The light management system further comprises an array of power units disposed on a front surface of the electrochromic film stack, where each power unit comprises at least one solar microcell. Collectively, the solar microcells cover an area no greater than about 6% of a total area of the front surface. The array of power units is configured to control the charging and discharging of the electrochromic layer, thereby manipulating light transmission through the electrochromic film stack.
Yoder, Mikayla A.↗
Revisiting Conversion Reaction Mechanisms in Lithium Batteries: Lithiation-Driven Topotactic Transformation in FeF 2
Intercalation-type electrodes have now been commonly employed in today’s batteries as such materials are capable of storing and releasing lithium reversibly via topotactic transformation, conducive to small structural change, but they have limited interstitial sites to hold Li. In contrast, conversion electrodes feature high Li-storage capacity, but often undergo large structural change during (de)lithiation, resulting in cycling instability. One exception is iron fluoride (FeF 2 ), a conversion-type cathode that exhibits both high capacity and high cycling stability. Herein, we report a lithiation-driven topotactic transformation in a single crystal of FeF2, unveiled by in situ visualization of the spatial and crystallographic correlation between the parent and converted phases. Specifically, conversion in FeF 2 resembles the intercalation process but involves transport of both Li + and Fe 2+ ions within the F-anion array, leading to formation of Fe preferentially along specific crystallographic orientations of FeF 2 . Throughout the process, the F-anion framework is retained, creating a checkerboard-like structure, within which the volume change is largely compensated, thereby enabling the high cyclability in FeF 2 . Lastly, findings from this study, with unique insights into conversion reaction mechanisms, may help to pave the way for designing conversion-type electrodes for the next-generation high energy lithium batteries.
25 ENERGY STORAGE↗
Photoanodic behavior of vapor-liquid-solid–grown, lightly doped, crystalline Si microwire arrays
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solar (photovoltaic), solid state lighting, phonon↗
Domain-Matching Epitaxy of Ferroelectric Hf 0.5 Zr 0.5 O 2 (111) on La 2/3 Sr 1/3 MnO 3 (001)
Epitaxial ferroelectric HfO2 films are the most suitable to investigate intrinsic properties of the material and for prototyping emerging devices. Ferroelectric Hf 0.5 Zr 0.5 O 2 (111) films were epitaxially stabilized on La 2/3 Sr 1/3 MnO 3 (001) electrodes. This epitaxy, considering the symmetry dissimilarity and the huge lattice mismatch, is not compatible with conventional mechanisms of epitaxy. In this work, to gain insight into the epitaxy mechanism, scanning transmission electron microscopy characterization of the interface was performed, revealing arrays of dislocations with short periodicities. Additionally, these observed periodicities agree with those expected for domain matching epitaxy, indicating that this unconventional mechanism could be the prevailing factor in the stabilization of ferroelectric Hf0.5Zr0.5O2 with (111) orientation in the epitaxial Hf 0.5 Zr 0.5 O 2 (111)/La 2/3 Sr 1/3 MnO 3 (001)heterostructure.
36 MATERIALS SCIENCE↗
Editors’ Choice—Review—Recent Advances in Mixed Potential Sensors
Gas sensors are widely used in environmental monitoring and provide controls especially when working with toxic gases. YSZ based λ-sensors have been utilized in the automobile industry for exhaust gas monitoring for more than 40 years. However, recent regulations on emissions reduction has forced further development of toxic gases monitoring in various applications. Mixed potential sensors with YSZ electrolyte are receiving increased attention due to their higher sensitivity and durability under harsh conditions. This review focuses on recent (past 5 years) developments made on electrode and electrolyte structure along with new sensing electrode materials towards detecting gases such as NO x , NH 3 , H 2 , CO and hydrocarbons (HCs). The theory of mixed potential sensors is discussed along with recent developments in detection of multi-gas mixtures using the output from an array of sensors in a mathematical model. Future directions for mixed potential sensor research, and methodologies to improving sensing characteristics are also outlined
47 OTHER INSTRUMENTATION↗
Remote-Contact Catalysis for Target-Diameter Semiconducting Carbon Nanotube Arrays
Electrostatic catalysis has been an exciting development in chemical synthesis (beyond enzymes catalysis1 ) in recent years, boosting reaction rates and selectively producing certain reaction products2 . Most of the studies to date have been focused on using external electric field (EEF) to rearrange the charge distribution in small molecule reactions such as Diels-Alder addition3 , carbene reaction4 , etc. However, in order for these EEFs to be effective, a field on the order of 1 V/nm (10 MV/cm) is required, and the direction of the EEF has to be aligned with the reaction axis5 . Such a large and oriented EEF will be challenging for large-scale implementation, or materials growth with multiple reaction axis or steps. Here, we demonstrate that the energy band at the tip of an individual single-walled carbon nanotube6 (SWCNT) can be spontaneously shifted in a high-permittivity growth environment, with its other end in contact with a low-work function electrode (e.g., hafnium carbide or titanium carbide7 ). By adjusting the Fermi level at a point where there is a substantial disparity in the density of states (DOS) between semiconducting (s-) and metallic (m-) SWCNTs8 , we achieve effective electrostatic catalysis for s-SWCNT growth assisted by a weak EEF perturbation (200V/cm). This approach enables the production of high-purity (99.92%) s-SWCNT horizontal arrays with narrow diameter distribution (0.95±0.04 nm), targeting the requirement of advanced SWCNT-based electronics for future computing9-11. These findings highlight the potential of electrostatic catalysis in precise materials growth, especially for s-SWCNTs, and pave the way for the development of advanced SWCNT-based electronics12.
Wang, Jiangtao↗
Circuit model of the ITER-like antenna for JET and simulation of its control algorithms
The ITER-like Antenna (ILA) for JET [1] is a 2 toroidal by 2 poloidal array of Resonant Double Loops (RDL) featuring in-vessel matching capacitors feeding RF current straps in conjugate-T manner, a low impedance quarter-wave impedance transformer, a service stub allowing hydraulic actuator and water cooling services to reach the aforementioned capacitors and a 2nd stage phase-shifter-stub matching circuit allowing to correct/choose the conjugate-T working impedance. Toroidally adjacent RDLs are fed from a 3dB hybrid splitter. It has been operated at 33, 42 and 47MHz on plasma (2008-2009) while it presently estimated frequency range is from 29 to 49MHz. At the time of the design (2001-2004) as well as the experiments the circuit models of the ILA were quite basic. The ILA front face and strap array Topica model was relatively crude and failed to correctly represent the poloidal central septum, Faraday Screen attachment as well as the segmented antenna central septum limiter. The ILA matching capacitors, T-junction, Vacuum Transmission Line (VTL) and Service Stubs were represented by lumped circuit elements and simple transmission line models. The assessment of the ILA results carried out to decide on the repair of the ILA identified that achieving routine full array operation requires a better understanding of the RF circuit, a feedback control algorithm for the 2nd stage matching as well as tighter calibrations of RF measurements. The paper presents the progress in modelling of the ILA comprising a more detailed Topica model of the front face for various plasma Scrape Off Layer profiles, a comprehensive HFSS model of the matching capacitors including internal bellows and electrode cylinders, 3D-EM models of the VTL including vacuum ceramic window, Service stub, a transmission line model of the 2nd stage matching circuit and main transmission lines including the 3dB hybrid splitters. A time evolving simulation using the improved circuit model allowed to design and simulate the effectiveness of a feedback control algorithm for the 2nd stage matching and demonstrates the simultaneous matching and control of the 4 RDLs: 11 feedback loops control 21 actuators (8 capacitors, 4 phase shifters and 4 stubs for the 2nd stage matching, 4 main phase shifters controlling of the toroidal phasing and the electronically controlled phase between RF sources feeding top and bottom parts of the array and determines the poloidal phasing of the array which is solved explicitly at each time step) on (simulated) ELMy plasmas.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Three Dimensional Indium–Tin-Oxide Nanorod Array for Charge Collection in Dye-Sensitized Solar Cells
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bio-inspired↗
Light Harvesting Arrays of Polypyridine Ruthenium(II) Chromophores Prepared by Reversible Addition–Fragmentation Chain Transfer Polymerization
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catalysis (heterogeneous)↗
High spatial resolution direct conversion amorphous selenium X-ray detectors with monolithically integrated CMOS readout
Recent progress in the field of micron-scale spatial resolution direct conversion X-ray detectors for high-energy synchrotron light sources serve applications ranging from nondestructive and noninvasive microscopy techniques which provide insight into the structure and morphology of crystals, to medical diagnostic measurement devices. Amorphous selenium ( a -Se) as a wide-bandgap thermally evaporated photoconductor exhibits ultra-low thermal generation rates for dark carriers and has been extensively used in X-ray medical imaging. Being an amorphous material, it can further be deposited over large areas at room temperatures and at substantially lower costs as compared to crystalline semiconductors. Here, to address the demands for a high-energy and high spatial resolution X-ray detector for synchrotron light source applications, we have thermally evaporated a -Se on a Mixed-Mode Pixel Array Detector (MM-PAD) Application Specific Integrated Circuit (ASIC). The ASIC format consists of 128 × 128 square pixels each 150 μm on a side. A 200 μm a -Se layer was directly deposited on the ASIC followed by a metal top electrode. The completed detector assembly was tested with 45 kV Ag and 23 kV Cu X-ray tube sources. The detector fabrication, performances, Modulation Transfer Function (MTF) measurements, and simulations are reported.
36 MATERIALS SCIENCE↗
Dynamic imaging of metastable reaction pathways in lithiated cobalt oxide electrodes
Understanding how lithium-ion batteries function down to the atomic level during charge and discharge cycling can provide valuable guidance to optimize structure-property relationships and to design and understand new electrode materials. Lithium insertion and reactions with the electrodes during charge and discharge cycling can occur via metastable structures with complex ordering and related non-equilibrium phenomena. Remarkably, these processes remain still poorly understood despite their significance in the operation of lithium battery systems in critical technologies. In this communication, we present the dynamics of lithium insertion into Co3O4 and the evolution of metastable phases as probed by in-situ transmission electron microscopy, in concert with first principles density functional theory calculations. We show that the initial lithium intercalation reaction occurs with the formation of several metastable and intermediate phases, followed by a sequence of conversion reactions that perturb and expand the cubic-close-packed oxygen array, ultimately generating an end-product of finely dispersed cobalt metal clusters within a Li2O matrix. The calculated non-equilibrium lithiation pathways corroborate with the experimental lithiation voltages, and explain the significant hysteresis that occurs during electrochemical cycling. The data provide new insights into the complexity of solid state lithium electrochemistry in metal oxides that are relevant to advancing lithium battery technology.
conversion reaction electrode↗
Reaction Diffusion Modelling of 3D Pillar Electrodes in Single-Catalyst CO 2 Reduction Cascades
Effective electrochemical CO 2 reduction to liquid fuels requires that the local catalytic environment facilitates the desired reactivity, yet a microscopic understanding of this environment is difficult to achieve from experiment alone. In this work, a 3D reaction-diffusion model was developed to explore the effects of electrode surface area and local geometry on the performance of a heterogeneous catalyst that performs a two-step CO 2 reduction cascade reaction to CO and then CH 3 OH under aqueous conditions. Kinetic parameters for the model were inspired by experimental results using a cobalt phthalocyanine (CoPc) catalyst. Three-dimensional architectures composed of arrays of square pillars with varying dimensions and either smooth or periodically modulated surfaces were tested, revealing the extent to which geometry modulates the performance of the cascade reactions. Although structural variations modulate local concentration gradients, we find that electrochemically active surface area predominantly governs the overall cascade reaction. Moreover, the results suggest that supersaturation of CO, with concentrations up to ten-fold higher than the equilibrium solubility limit, might be critical for more efficient conversion to CH 3 OH. For any given geometry, the spatially averaged ratio of [CO] to [CO 2 ] is dictated by the electrochemically active surface area and determines the yield of CH 3 OH. For a fixed surface area, geometries that spatially confine the electrolyte yield moderate local [CO] to [CO 2 ] ratios within small volumes. In contrast, less confining geometries result in a broader distribution of local ratios spread over larger volumes, with both configurations yielding the same spatially averaged [CO] to [CO 2 ] ratio. These insights provide valuable design principles—highlighting the critical importance of surface area and possibly CO supersaturation—for engineering advanced electrode architectures that leverage intermediate trapping and CO supersaturation to enhance overall performance in tandem CO 2 reduction systems.
COMSOL↗
Single occupancy spectroelectrochemistry of freely diffusing flavin mononucleotide in zero-dimensional nanophotonic structures
Zero-mode waveguides (ZMW) have the potential to be powerful confinement tools for studying electron transfer dynamics at single molecule occupancy conditions. Flavin mononucleotide contains an isoalloxazine chromophore, which is fluorescent in the oxidized state (FMN) while the reduced state (FMNH 2 ) exhibits dramatically lower light emission, i.e. a dark-state. This allows fluorescence emission to report the redox state of single FMN molecules, an observation that has been used previously to study single electron transfer events in surface-immobilized flavins and flavoenzymes, e.g. sarcosine oxidase, by direct wide-field imaging of ZMW arrays. Single molecule electron transfer dynamics have now been extended to the study of freely diffusing molecules using fluorescence measurements of Au ZMWs under single occupancy conditions. The Au in the ZMW serves both as an optical cladding layer and as the working electrode for potential control, thereby accessing single molecule electron transfer dynamics at μM concentrations. Consistent with expectations, the probability of observing single reduced molecules increases as the potential is scanned negative, E appl < E eq , and the probability of observing emitting oxidized molecules increases at E appl > E eq . Different single molecules exhibit different electron transfer properties as reflected in the position of E eq and the distribution of E eq among a population of FMN molecules. Two types of actively-controlled electroluminescence experiments were used: chronofluorometry experiments, in which the potential is alternately stepped between oxidizing and reducing potentials, and cyclic potential sweep fluorescence experiments, analogous to cyclic voltammetry, these latter experiments exhibiting a dramatic scan rate dependence with the slowest scan rates showing distinct intermediate states that are stable over a range of potentials. These states are assigned to flavosemiquinone species that are stabilized in the special environment of the ZMW nanopore.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗