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DOE OSTI2014

SU-D-19A-01: Can Farmer-Type Ionization Chambers Be Used to Improve the Accuracy of Low-Energy Electron Beam Reference Dosimetry?

Purpose: To investigate the use of cylindrical Farmer-type ionization chambers to improve the accuracy of low-energy electron beam calibration. Historically, these chamber types have not been used in beams with incident energies less than 10 MeV (R{sub 5} {sub 0} < 4.3 cm) because early investigations suggested large (up to 5 %) fluence perturbation factors in these beams, implying that a significant component of uncertainty would be introduced if used for calibration. More recently, the assumptions used to determine perturbation corrections for cylindrical chambers have been questioned. Methods: Measurements are made with cylindrical chambers in Elekta Precise 4, 8 and 18 MeV electron beams. Several chamber types are investigated that employ graphite walls and aluminum electrodes with very similar specifications (NE2571, NE2505/3, FC65-G). Depth-ionization scans are measured in water in the 8 and 18 MeV beams. To reduce uncertainty from chamber positioning, measurements in the 4 MeV beam are made at the reference depth in Virtual Water™. The variability of perturbation factors is quantified by comparing normalized response of various chambers. Results: Normalized ion chamber response varies by less than 0.7 % for similar chambers at average electron energies corresponding to that at the reference depth from 4 or 6 MeV beams. Similarly, normalized measurements made with similar chambers at the reference depth in the 4 MeV beam vary by less than 0.4 %. Absorbed dose calibration coefficients derived from these results are stable within 0.1 % on average over a period of 6 years. Conclusion: These results indicate that the uncertainty associated with differences in fluence perturbations for cylindrical chambers with similar specifications is only 0.2 %. The excellent long-term stability of these chambers in both photon and electron beams suggests that these chambers might offer the best performance for all reference dosimetry applications.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2022

Anion Effects on the Interfacial Structure and Bulk Physical Properties in Choline-Based Hydrogen-Bonded Electrolytes

Electrolytes consisting of choline (Ch) salts with acetate (Ac) and oxalate (Ox) anions were studied in mixtures with ethylene glycol (EG), in comparison to chloride (Cl)- and bis(trifluorosulfonyl)imide (TFSI)-containing systems to understand the impact of anion size and charge density on the bulk electrolyte and interfacial properties. These represent hydrogen-bonded concentrated electrolytes where the Ch salts are the H-bond acceptors (HBAs) and EG is the H-bond donor (HBD) in 1:2 and 1:4 HBA:HBD ratios. Increased H-bonding in Ch 2 Ox with EG compacts the liquid compared to ChAc, consistent with the increased dissociation energies of the HBA:HBD clusters with Ox –2 calculated by density functional theory (DFT), thus leading to denser and more viscous liquids. Electrochemical impedance spectroscopy (EIS) and surface-enhanced Raman spectroscopy (SERS) were used to investigate interfacial charge density and the electrode surface species. Differential capacitance curves demonstrate weak dependence on potential except for ChAc:EG, where Ac – is found to adsorb on the Au surface, in particular at +0.055 V vs Ag quasi-reference while no specific adsorption was observed on glassy carbon (GC). In situ SERS measurement confirms the formation of a surface layer in the ChAc:EG systems resulting from a Au–acetate interaction. Despite the structural similarities, Ox –2 did not show specific binding or any dependence of capacitance on potential as a result of strongly solvating EG molecules via H-bonds. Furthermore, this study shows that the charge density of the HBAs impacts both bulk properties and the electrical double-layer formation in concentrated H-bonded electrolytes that is relevant to electrochemical kinetics and morphology in electrodeposition processes and energy storage applications.

25 ENERGY STORAGE↗

DOE OSTI2014

Photon assisted current in molecular nanojunctions with novel types of contacts

We propose new approaches to coherent control of transport via molecular junctions, which bypasses several of the hurdles to experimental realization of optically manipulated nanoelectronics noted in the previous literature. The first method is based on the application of intrinsic semiconductor contacts and optical frequencies below the semiconductor bandgap. Our analytical theory predicts a new phenomenon, referred to as coherent destruction of induced tunnelling, which extends the phenomenon of coherent destruction of tunnelling frequently discussed in the previous literature. We also propose to use graphene electrodes as a platform for effective photon assisted tunneling through molecular conduction nanojunctions. We predict dramatic increasing currents evaluated at side-band energies ∼nħω (n is a whole number) related to the modification of graphene gapless spectrum under the action of external electromagnetic field of frequency ω. Our results illustrate the potential of semiconductor and graphene contacts in coherent control of photocurrent.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Ternary alkali-metal and transition metal or metalloid acetylides as alkali-metal intercalation electrodes for batteries

Novel intercalation electrode materials including ternary acetylides of chemical formula: A.sub.nMC.sub.2 where A is alkali or alkaline-earth element; M is transition metal or metalloid element; C.sub.2 is reference to the acetylide ion; n is an integer that is 0, 1, 2, 3 or 4 when A is alkali element and 0, 1, or 2 when A is alkaline-earth element. The alkali elements are Lithium (Li), Sodium (Na), Potassium (K), Rubidium (Rb), Cesium (Cs) and Francium (Fr). The alkaline-earth elements are Berilium (Be), Magnesium (Mg), Calcium (Ca), Strontium (Sr), Barium (Ba), and Radium (Ra). M is a transition metal that is any element in groups 3 through 12 inclusive on the Periodic Table of Elements (elements 21 (Sc) to element 30 (Zn)). In another exemplary embodiment, M is a metalloid element.

25 ENERGY STORAGE↗

DOE OSTI2026

Cryogenic light detectors with thermal signal amplification for 0 νββ search experiments

As a step towards the realization of cryogenic-detector experiments to search for neutrinoless double-beta decay (such as CROSS, BINGO, and CUPID), we investigated a batch of 10 Ge light detectors (LDs) assisted by Neganov-Trofimov-Luke (NTL) signal amplification. Each LD was assembled with a large cubic light-emitting crystal (45 mm side) using the recently developed CROSS mechanical structure. The detector array was operated at milli-Kelvin temperatures in a pulse-tube cryostat at the Canfranc underground laboratory in Spain. We achieved good performance with scintillating bolometers from CROSS, made of Li 2 100 MoO 4 crystals and used as reference detectors of the setup, and with all LDs tested (except for a single device that encountered an electronics issue). No leakage current was observed for 8 LDs with an electrode bias up to 100 V. Operating the LDs at an 80 V electrode bias applied in parallel, we obtained a gain of around 9 in the signal-to-noise ratio of these devices, allowing us to achieve a baseline noise RMS of O(10 eV). Thanks to the strong current polarization of the temperature sensors, the time response of the devices was reduced to around half a millisecond in rise time. The achieved performance of the LDs was extrapolated via simulations of pile-up rejection capability for several configurations of the CUPID detector structure. Despite the sub-optimal noise conditions of the LDs (particularly at high frequencies), we demonstrated that the NTL technology provides a viable solution for background reduction in CUPID.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Methods—Kintsugi Imaging of Battery Electrodes: Distinguishing Pores from the Carbon Binder Domain using Pt Deposition

The mesostructure of porous electrodes used in lithium-ion batteries strongly influences cell performance. Accurate imaging of the distribution of phases in these electrodes would allow this relationship to be better understood through simulation. However, imaging the nanoscale features in these components is challenging. While scanning electron microscopy is able to achieve the required resolution, it has well established difficulties imaging porous media. This is because the flat imaging planes prepared using focused ion beam milling will intersect with the pores, which makes the images hard to interpret as the inside walls of the pores are observed. It is common to infiltrate porous media with resin prior to imaging to help resolve this issue, but both the nanoscale porosity and the chemical similarity of the resins to the battery materials undermine the utility of this approach for most electrodes. In this study, a technique is demonstrated which uses in situ infiltration of platinum to fill the pores and thus enhance their contrast during imaging. Reminiscent of the Japanese art of repairing cracked ceramics with precious metals, this technique is referred to as the kintsugi method. The images resulting from applying this technique to a conventional porous cathode are presented and then segmented using a multi-channel convolutional method. We show that while some cracks in active material particles were empty, others appear to be filled (perhaps with the carbon binder phase), which will have implications for the rate performance of the cell. Energy dispersive X-ray spectroscopy was used to validate the distribution of phases resulting from image analysis, which also suggested a graded distribution of the binder relative to the carbon additive. The equipment required to use the kintsugi method is commonly available in major research facilities and so we hope that this method will be rapidly adopted to improve the imaging of electrode materials and porous media in general.

25 ENERGY STORAGE↗

DOE OSTI2018

Physical Reasoning to Synchronize Electrical Signals and Related Diagnostics in Plasma Focus Devices

Plasma Focus (PF) devices as well as other similar pulsed discharge devices requires a variety of diagnostics for their proper control and optimization, including the voltage between electrodes, the time derivative of the discharge current, detection of X-rays and neutron emissions, and pulsed laser images (Shadow, Schlieren, interferograms). This article discusses the problem of the time reference of all these outputs and proposes specific techniques for synchronizing them based on sound physical grounds. The foundations of synchronization criterion are verified in several experiments on PF devices.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS2004

Automatic Control of Arc Process for Making Carbon Nanotubes

An automatic-control system has been devised for a process in which carbon nanotubes are produced in an arc between a catalyst-filled carbon anode and a graphite cathode. The control system includes a motor-driven screw that adjusts the distance between the electrodes. The system also includes a bridge circuit that puts out a voltage proportional to the difference between (1) the actual value of potential drop across the arc and (2) a reference value between 38 and 40 V (corresponding to a current of about 100 A) at which the yield of carbon nanotubes is maximized. Utilizing the fact that the potential drop across the arc increases with the interelectrode gap, the output of the bridge circuit is fed to a motor-control circuit that causes the motor to move the anode toward or away from the cathode if the actual potential drop is more or less, respectively, than the reference potential. Thus, the system regulates the interelectrode gap to maintain the optimum potential drop. The system also includes circuitry that records the potential drop across the arc and the relative position of the anode holder as function of time.

Scott, Carl D.↗

DOE OSTI2018

Origins and Implications of Interfacial Capacitance Enhancements in C 60 -Modified Graphene Supercapacitors

Understanding and controlling the electrical response at a complex electrode–electrolyte interface is key to the development of next-generation supercapacitors and other electrochemical devices. In this work, we apply a theoretical framework based on the effective screening medium and reference interaction site model to explore the role of electrical double-layer (EDL) formation and its interplay with quantum capacitance in graphene-based supercapacitors. In addition to pristine graphene, we investigate a novel C60-modified graphene supercapacitor material, which promises higher charge-storage capacity. Beyond the expected enhancement in the quantum capacitance, we find that the introduction of C60 molecules significantly alters the EDL response. These changes in EDL are traced to the interplay between surface morphology and charge localization character and ultimately dominate the overall capacitive improvement in the hybrid system. Our study highlights a complex interplay among surface morphology, electronic structure, and interfacial capacitance, suggesting general improvement strategies for optimizing carbon-based supercapacitor materials.

36 MATERIALS SCIENCE↗

NASA NTRS1971

Development of improved pyroelectric detectors; Literature survey of pyroelectric materials and their characteristics

The object of this program is to improve the detectivity of the pyroelectric detector with the ultimate goal of operation at or near the temperature-noise limit. Two general areas of investigation are undertaken. The first is to improve responsivity through the use of new materials. The second is directed toward reduction of noise and will be effected with improved field effect transistor characteristics, and improved electroding of the pyroelectric material. The search for new materials has begun with a review of the literature on pyroelectric materials in several languages. The compiled data includes an extensive list of references. From this, several materials have already been selected for investigation. FETs are being obtained from various manufacturers, evaluated, and selected units will be tested with pyroelectric elements as complete detectors.

Weiner, S.↗

DOE OSTI2024

FET Junction Temperature Monitoring Using Novel On-Chip Solution

A novel junction temperature monitoring sensor is proposed and experimentally demonstrated for application in MOS-gate power devices. The sensor is created using the polycide gate electrode layer of the devices to create a temperature-sensitive resistor without any additional fabrication steps. The resistor is located on the field oxide with one end grounded at the device reference terminal to isolate it from the device current and voltage transients. It allows in-situ monitoring of the device junction temperature during active circuit operation. The technology has been implemented to monitor the junction temperature of Silicon Carbide Junction Barrier Schottky Field Effect Transistors (SiC JBSFETs) with the bi-directional FET (BiDFET).

Bidirectional switches, SiC bidirectional FET, BiD↗

DOE OSTI2014

Asynchronous Stoichiometric Response in Lithium Iron Phosphate Batteries

The operando energy-dispersive x-ray diffraction (EDXRD) was carried out on a newly formed 8 Ah lithium iron phosphate (LiFePO4) battery with the goal of elucidating the origin of asynchronous phase transformation commonly seen with in situ x-ray diffraction studies. The high-energy photons at the NSLS X17B1 beamline allow for penetration into a fully assembled battery and therefore negate any need for a specially designed in situ cell which often uses modified current collectors to minimize x-ray attenuation. Spatially-and-temporally resolved phase-mapping was conducted with a semiquantitative reference intensity ratio (RIR) analysis to estimate the relative abundance of the delithiated phase. The data show an asynchronous response in the stoichiometry versus the electrochemical profile and suggest limited diffusion in the electrode toward the end of discharge. These results confirm that the asynchronous electrode response is not just limited to specially designed cells but occurs in fully assembled cells alike. We attribute this behavior to be a consequence of performing a local measurement over a wide-area heterogeneous reaction.

25 ENERGY STORAGE↗

NASA NTRS1977

Investigation of possible lower hybrid emission from the NASA Lewis Bumpy Torus plasma

Radio frequency emission detected near the lower hybrid frequency of the NASA Lewis Bumpy Torus plasma is studied, using a simple detection system that consists of a spectrum analyzer and a 50-ohm miniature co-axial antenna concentrically located in a re-entrant quartz tube. The frequency shift of a broad emission peak is monitored as a function of the background pressure, electrode voltage, and the strength of the dc magnetic field. Simultaneous measurements of the average plasma density are made with a polarization diplexing microwave interferometer. Information from the experiment is discussed with particular reference to the role of atomic or molecular species of deuterium in the emissions, the strength of the dc magnetic field in the emitting region, the geometric location of the emitting region of the plasma, the lower hybrid plasma density as compared with the average plasma density, and the relation of the ion spoke geometry to the lower hybrid emission.

Mallavarpu, R.↗

NASA NTRS1978

Some studies on a solid-state sulfur probe for coal gasification systems

As a part of a program for the development of a sulfur probe for monitoring the sulfur potential in coal gasification reactors, an investigation was conducted regarding the efficiency of the solid electrolyte cell Ar+H2+H2S/CaS+CaF2+(Pt)//CaF2//Pt)+CaF2+CaS/H2S+H2+Ar. A demonstration is provided of the theory, design, and operation of a solid-state sulfur probe based on CaF2 electrolyte. It was found that the cell responds to changes in sulfur potential in a manner predicted by the Nernst equation. The response time of the cell at 1225 K, after a small change in temperature or gas composition, was 2.5 Hr, while at a lower temperature of 990 K the response time was approximately 9 hr. The cell emf was insensitive to a moderate increase in the flow rate of the test gas and/or the reference gas. The exact factors affecting the slow response time of galvanic cells based on a CaF2 electrolyte have not yet been determined. The rate-limiting steps may be either the kinetics of electrode reactions or the rate of transport through the electrolyte.

Jacob, K. T.↗

DOE OSTI2018

Interphases in Sodium-Ion Batteries

Sodium-ion batteries (SIBs) as economical high energy alternatives to lithium-ion batteries (LIBs) have received significant attention for large-scale energy storage in the last few years. While the efforts of developing SIBs have benefited from the knowledge learned in LIBs, thanks to the apparent proximity between Na-ion and Li-ion, the unique physical and chemical properties of Na-ion also distinctly differ itself from Li-ion. It is expected SIBs have drastically different electrode material structure, solvation-de-solvation behavior, electrode-electrolyte interphase stability, ion transfer property, and hence electrochemical performance of batteries. In this review, we comprehensively summarize the current understanding of the anode solid-electrolyte-interphase (SEI) and cathode cathode-electrolyte-interphase (CEI) in SIBs, with an emphasis on how the tuning of the stability and ion transfer properties of interphases fundamentally determines the reversibility and efficiency of electrochemical reactions. Through these carefully screened references, we intend to reveal the intrinsic correlation between the properties/functionalities of the interphases and the electrochemical performances of batteries.

Song, Junhua↗

DOE OSTI2024

A thermodynamic perspective on electrode poisoning in solid oxide fuel cells

A critical challenge to the commercialization of clean and high-efficiency solid oxide fuel cell (SOFC) technology is the insufficient stack lifespan caused by a variety of degradation mechanisms, which are associated with cell components and chemical feedstocks. Cell components related degradation refers to thermal/chemical/electrochemical deterioration of cell materials under operating conditions, whereas the latter regards impurities in feedstocks of oxidant (air) and reductant (fuel). This article provides a thermodynamic perspective on the understanding of the impurities-induced degradation mechanisms in SOFCs. The discussion focuses on using thermodynamic analysis to elucidate poisoning mechanisms in cathodes by impurity species such as Cr, CO 2 , H 2 O, and SO 2 and in the anode by species such as S (or H 2 S), SiO 2 , and P 2 (or PH 3 ). The author hopes the presented fundamental insights can provide a theoretical foundation for searching for better technical solutions to address the critical degradation challenges.

25 ENERGY STORAGE↗

DOE OSTI2016

SU-C-201-03: Ionization Chamber Collection Efficiency in Pulsed Radiation Fields of High Pulse Dose

Purpose: To investigate the reduction of collection efficiency of ionization chambers (IC) by volume recombination and its correction in pulsed fields of very high pulse dose. Methods: Measurements of the collection efficiency of a plane-parallel advanced Markus IC (PTW 34045, 1mm electrode spacing, 300V nominal voltage) were obtained for collection voltages of 100V and 300V by irradiation with a pulsed electron beam (20MeV) of varied pulse dose up to approximately 600mGy (0.8nC liberated charge). A reference measurement was performed with a Faraday cup behind the chamber. It was calibrated for the liberated charge in the IC by a linear fit of IC measurement to reference measurement at low pulse doses. The results were compared to the commonly used two voltage approximation (TVA) and to established theories for volume recombination, with and without considering a fraction of free electrons. In addition, an equation system describing the charge transport and reactions in the chamber was solved numerically. Results: At 100V collection voltage and moderate pulse doses the established theories accurately predict the observed collection efficiency, but at extreme pulse doses a fraction of free electrons needs to be considered. At 300V the observed collection efficiency deviates distinctly from that predicted by any of the established theories, even at low pulse doses. However, the numeric solution of the equation system is able to reproduce the measured collection efficiency across the entire dose range of both voltages with a single set of parameters. Conclusion: At high electric fields (3000V/cm here) the existing theoretical descriptions of collection efficiency, including the TVA, are inadequate to predict pulse dose dependency. Even at low pulse doses they might underestimate collection efficiency. The presented, more accurate numeric solution, which considers additional effects like electric shielding by the charges, might provide a valuable tool for future investigations. This project was funded by the German ministry of research and education (BMBF) under grant number: 03Z1N511 and by the state of Saxony under grant number: B 209.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1977

Investigation of possible lower hybrid emission from the NASA Lewis bumpy torus plasma

Radio frequency emission has been detected near the power hybrid frequency of a bumpy torus plasma by using a responsive detection system that consists of a spectrum analyzer and a 50 ohm miniature coaxial antenna concentrically located in a re-entrant quartz tube. The frequency shift of a broad emission peak was monitored as a function of background pressure, electrode voltage, and the strength of the dc magnetic field. Simultaneous measurements of the average plasma density were made with a polarization diplexing microwave interferometer. The information derived from the experiment is discussed with particular reference to the following: (1) whether the emissions are dominated by atomic or molecular species of deuterium; (2) the strength of the dc magnetic field in the emitting region; (3) the geometric location of the emitting region of the plasma; (4) comparison of the lower hybrid plasma density with the average plasma density; and (5) relation of ion spoke geometry to lower hybrid emission.

Mallavarpu, R.↗