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DOE OSTI2016

The mechanical design and simulation of a scaled H{sup −} Penning ion source

The existing ISIS Penning H{sup −} source is unable to produce the beam parameters required for the front end test stand and so a new, high duty factor, high brightness scaled source is being developed. This paper details first the development of an electrically biased aperture plate for the existing ISIS source and second, the design, simulation, and development of a prototype scaled source.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2015

Size scaling of negative hydrogen ion sources for fusion

The RF-driven negative hydrogen ion source (H{sup −}, D{sup −}) for the international fusion experiment ITER has a width of 0.9 m and a height of 1.9 m and is based on a ⅛ scale prototype source being in operation at the IPP test facilities BATMAN and MANITU for many years. Among the challenges to meet the required parameters in a caesiated source at a source pressure of 0.3 Pa or less is the challenge in size scaling of a factor of eight. As an intermediate step a ½ scale ITER source went into operation at the IPP test facility ELISE with the first plasma in February 2013. The experience and results gained so far at ELISE allowed a size scaling study from the prototype source towards the ITER relevant size at ELISE, in which operational issues, physical aspects and the source performance is addressed, highlighting differences as well as similarities. The most ITER relevant results are: low pressure operation down to 0.2 Pa is possible without problems; the magnetic filter field created by a current in the plasma grid is sufficient to reduce the electron temperature below the target value of 1 eV and to reduce together with the bias applied between the differently shaped bias plate and the plasma grid the amount of co-extracted electrons. An asymmetry of the co-extracted electron currents in the two grid segments is measured, varying strongly with filter field and bias. Contrary to the prototype source, a dedicated plasma drift in vertical direction is not observed. As in the prototype source, the performance in deuterium is limited by the amount of co-extracted electrons in short as well as in long pulse operation. Caesium conditioning is much harder in deuterium than in hydrogen for which fast and reproducible conditioning is achieved. First estimates reveal a caesium consumption comparable to the one in the prototype source despite the large size.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Ring-opening and hydrodenitrogenation of indole under hydrothermal conditions over Ni, Pt, Ru, and Ni-Ru bimetallic catalysts

Here, the activity and selectivity of activated-carbon-supported Ni, Pt, Ru, and Ni-Ru bimetallic catalysts was examined for hydrothermal denitrogenation of indole. The molar yield of pyrrole ring-opening compounds, without an added hydrogen source, are in the order: Ni < Pt < Ni 90 Ru 10 < Ni 75 Ru 25 < Ni 50 Ru 50 ~ Ni 25 Ru 75 ~ Ru. Ru-containing catalysts facilitated production of hydrocarbons (hydrodenitrogenation (HDN) products) when used with added formic acid (hydrogen source). We elucidated catalytic hydrothermal HDN pathways for indole based on the product distributions and the variation of their yields with time. Hydrogenation of indole to indoline is the primary pathway and ring-opening of indoline to form alkyl anilines is faster than forming HDN products (alkyl benzenes). DFT calculations confirmed experimental activity trends, showing Ru is more active than Ni for indole ring opening and for o-toluidine deamination. If no hydrogen source is present, directly breaking the N-C bond in the pyrrole ring is more favorable than breaking the C-N bond with an aromatic carbon. If a H source is provided, the pyrrole ring hydrogenates first, forming indoline, followed by cleavage of the C-N bond.

42 ENGINEERING↗

DOE OSTI2017

Effect of the SiO 2 interlayer properties with solid-source hydrogenation on passivated contact performance and surface passivation

We investigate how SiO x oxide interlayers prepared by different techniques (chemical, thermal) in combination with hydrogen released from an ALD Al 2 O 3 source layer govern passivation in 1) passivated contacts based on doped poly-Si layers and tunneling SiO 2 , and 2) wafer surface passivation by Al 2 O 3 . Profiles of O and H in these structures with engineered, buried SiOx interlayers were measured by Time-of-Flight SIMS (TOF-SIMS) at nanometer resolution. Passivated contacts perform best with thermally oxidized SiOx, while chemical SiO x causes poly-Si film blistering and performance degradation. ALD Al 2 O 3 acts as passivating H source, significantly improving B-doped and intrinsic poly-Si contacts for IBC cells. Fast-diffusing hydrogen from the Al 2 O 3 source layer appears to penetrate Si wafer thickness, improving the passivation of structures at the opposite side. In contrast to the passivated contacts, chemical SiOx interlayer promotes wafer surface passivation by ALD Al 2 O 3 , while similarly thin thermal SiO 2 suppresses passivation and built-in charge.

14 SOLAR ENERGY↗

NASA NTRS1992

A distance determination for the supernova remnant G27.4+0.0 and its central X-ray source

We have determined the distance to the supernova remnant G27.4+0.0, one of the handful of remnants with a bright central X-ray source. H I absorption data obtained with the VLA toward the remnant and adjacent H II regions allow us to constrain the distance to G27.4+0.0 to lie between 6 and 7.5 kpc. We briefly discuss the implications of this result for the nature of the central source.

Sanbonmatsu, K. Y.↗

DOE OSTI2016

Balmer-α spectrum measurements of the LHD one-third ion source

Wavelength spectra of Balmer-α light from plasmas in the extraction region of the Large Helical Device-R&D negative ion source, or the LHD one-third ion source have exhibited a blue shift as a negative bias voltage was applied to the plasma grid. The blue shift increased as the negative bias voltage with respect to the local plasma potential was increased. The measured spectra were compared with the velocity distributions of surface reflected hydrogen atoms calculated by atomic collisions in amorphous target code. The arc power and the source H{sub 2} pressure also affected the shift and broadening in the observed Balmer-α spectra. The possibility of identifying the negative hydrogen ions produced at the low work function plasma grid surface by high resolution spectroscopy is discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

Pre-conditioning procedure suitable for internal-RF-antenna of J-PARC RF-driven H{sup −} ion source

The Japan Proton Accelerator Research Complex (J-PARC) cesiated RF-driven H{sup −} ion source has been successfully operated for about 1 yr. By the world brightest level beam, the J-PARC design beam power of 1 MW was successfully demonstrated. Although no internal-RF-antenna failure, except for the once caused by an excess cesium due to a misoperation, occurred in the operation, many antennas failed in pre-conditionings for the first hundred days. The antenna failure rate was drastically decreased by using an antenna with coating thicker than a standard value and the pre-conditioning procedure repeating 15 min 25 kW RF-power operation and impurity-gas evacuation a few times, before the full power (50 kW) operation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

Fine-tuning to minimize emittances of J-PARC RF-driven H{sup −} ion source

The Japan Proton Accelerator Research Complex (J-PARC) cesiated RF-driven H{sup −} ion source has been successfully operated for about one year. By the world’s brightest level beam, the J-PARC design beam power of 1 MW was successfully demonstrated. In order to minimize the transverse emittances, the rod-filter-field (RFF) was optimized by changing the triple-gap-lengths of each of pairing five piece rod-filter-magnets. The larger emittance degradation seems to be caused by impurity-gases than the RFF. The smaller beam-hole-diameter of the extraction electrode caused the more than expected improvements on not only the emittances but also the peak beam intensity.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

The impact of second coordination sphere functional group extension on product selectivity for manganese bipyridyl CO 2 reduction electrocatalysts

Utilizing the well established manganese bipyridyl class of homogeneous electrocatalyst, four new ligands are studied to probe the influence of distal, outer coordination sphere, H-bonding and steric effects on product selectivity for proton-coupled electrocatalytic CO 2 reduction. The presence of a simple acetate functional group in the second coordination sphere provides a high selectivy for CO 2 -to-CO conversion irrespective of proton source (H 2 O vs. PhOH) or applied potential. The o-(methoxybenzoate)phenyl second/outer coordination sphere at the bipyridyl 6,6′-positions imparts poor product selectivity. In contrast, upon conjugation of the acetate functional group with the N-Boc-alanine moiety, a CO : HCO 2 − product selectivity of ∼1 : 1 is observed at the high overpotential catalytic wave (for both H 2 O and PhOH acids). Computed enthalpy and free energy of activation parameters suggest that selective CO 2 insertion at the manganese hydride transition state is favored, over protonation, consistent with negligible hydrogen production during controlled potential electrolysis studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2004

Removing Spectral Diagnostics of Galactic and Stellar X-Ray Emission from Charged Exchange Recombination

Our research uses the electron beam ion trap (EBIT) at the Lawrence Livermore National Laboratory to study X-ray emission from the charge exchange (CX) of highly charged ions with neutral gases. The resulting data help to fill a void in existing experimental and theoretical understanding of this atomic physics process, and are needed to explain all or part of the observed X-ray emission from the soft X-ray background, stellar winds, the Galactic Center and Galactic Ridge, supernova ejecta, and photoionized nebulae. Appreciation of the astrophysical relevance of our work continues to grow with the publication of roughly a dozen papers in the past four years describing Chandra and XMM observations of geocoronal and heliospheric CX emission, the temporal variation of such emission and correlation with X-ray emission enhancements observed by ROSAT, the theoretical spatial distribution of that emission, and CX emission around other stars. A similar number of papers were also published during that time describing CX emission from planets and comets. We expect that the launch of ASTRSE2, with its second-generation XRS microcalo- (with 6-eV resolution), will reveal even more clearly the contributions of CX to astrophysical emission. In our EBIT work we collected CX spectra from such ions as H-like and He-like Ne, Ar, and Fe. Our early measurements were made with a high-purity Ge detector, but during the second year we began operation of the first-generation XRS microcalorimeter (a twin of the XRS on ASTRO-E) and greatly improved the resolution of our measurements from roughly 150 eV (FWHM) with the Ge detectors to 10 eV with the XRS. We found that saturation of the XRS counting apparatus, which we described in our proposal as a potential concern, is not a problem for studying CX. During the course of our research, we expanded the number of injection gases permitted by the LLNL safety team, purchased and eventually operated an atomic H source, and clearly demonstrated the feasibility of our longer-range plan. For example, we successfully injected He into EBIT (not a small feat because of the difficulty of maintaining a good vacuum with He and avoiding electrical breakdown) to collect a H-like oxygen CX spectrum. The highest energy CX spectrum recorded with the XRS to date is that of the Ar K-shell emission. These measurements provided the first observation of the relative intensity ratios of resolved He-like singlet and triplet n=2->1 lines. We also carried out measurements of He-like Ne as a function of collision energy (i.e., ion temperature). Significant differences in the resulting x-ray spectra were noted. In all cases, the intensity of high-n H-like Lyman lines is significantly higher than current theoretical CX models predict.

Wargelin, Brad↗

NASA NTRS1979

Optical and X-ray properties of the newly discovered BL Lacertae object PKS 2155-304 /= H2155-304/

The soft X-ray source H 2155-304 has been precisely located with the HEAO 1 scanning modulation collimator, and identified with an object of bolometric magnitude approximately 14. The linear polarization, variability, spectrum, and diffuse image of the optical flux, together with the positional coincidence of the radio source PKS 2155-304, indicate that this object is a new member of the BL Lacertae class. Its characteristics are compared with those of other X-ray-emitting BL Lacertae objects, particularly Mrk 421.

Griffiths, R. E.↗

DOE OSTI2024

Hydrogen Storage for Load-Following and Clean Power: Duct-firing of Hydrogen to Improve the Capacity Factor of NGCC Plants (Final Report, Phase II Pre-Front End Engineering Design Study)

GTI Energy (GTI) and team members Southern Company Services (SCS), Pacific Gas & Electric (PG&E) and the Electric Power Research Institute (EPRI) performed a Phase II Pre-Feed Study under contract DE-FE0032008 for Hydrogen Storage for Load-Following and Clean Power. The configuration of the proposed system consists of subsystems for on-site H 2 production, on-site H 2 storage (up to 54 MWth in commercial vessels) and H 2 combustion in a duct burner in a Heat Recovery Steam Generator (HRSG) integrated with an existing fossil asset. Here, the firing rate of the duct burner is varied to let the plant respond to fluctuations of electrical load and H 2 production is relatively constant by storing H 2 . The proposed system is an improvement over alternate low carbon dispatchable power options. Technoeconomic analyses show H 2 produced with GTI’s patented Compact Hydrogen Generator (CHG) with inherent carbon capture will be lower cost (Levelized Cost of Hydrogen, LCOH) relative to hydrogen produced with a Steam Methane Reformer (SMR) with an amine system for carbon capture. This lower cost hydrogen enables our integrated system to deliver electricity (Levelized Cost of Electricity, LCOE) at 17.4% lower cost relative to a SMR sourced H 2 -fired HRSG (with an amine system for carbon capture) – Steam Turbine Generator (STG). Our analysis using EPRI’s US REGEN macroeconomic model shows our system will have significant demand in the power market and therefore require significant capacity expansion (CHG plants built to deliver hydrogen) to deliver low cost, low carbon power. In Phase II, our Team has completed a detailed system definition including the development of process models, definition of battery limits, Process Flow Diagrams (PFDs), Piping and Instrumentation Drawings (P&IDs), and a plant layout. A preliminary design for the key components of the CHG was developed including component lists & specifications. An evaluation of environmental and permitting considerations was completed and included the development of an Environmental Information Volume (EIV). The duct burners, which are flexible and can burn hydrogen and/or natural gas, were defined and initial CFD analyses were completed.

03 NATURAL GAS↗

NASA NTRS1987

A hard X-ray source in the nearest molecular cloud

The previous unidentified hard X-ray source H 0253 + 193 is coincident with Lynds 1457, a dark nebula at high galactic latitude (l = 159 deg, b = -34 deg). The Einstein IPC position coincides with the peak in the CO map obtained by Hobbs, Blitz, and Magnani (1986). Using interstellar Na I absorption, these authors determined a distance to the cloud of 65 pc, making this the nearest known molecular cloud. The X-ray source can be explained as an embedded T Tauri star with a 2-10 keV luminosity of 1 x 10 to the 31st erg/s.

Halpern, J. P.↗

DOE OSTI2025

Flow and thermal modelling of the argon volume in the DarkSide-20k TPC

The DarkSide-20k dark matter experiment, currently under construction at LNGS, features a dual-phase time projection chamber (TPC) with a ∼ 50 t argon target from an underground well. At this scale, it is crucial to optimise the argon flow pattern for efficient target purification and for fast distribution of internal gaseous calibration sources with lifetimes of the order of hours. To this end, we have performed computational fluid dynamics simulations and heat transfer calculations. The residence time distribution shows that the detector is well-mixed on time-scales of the turnover time (∼ 40 d). Notably, simulations show that despite a two-order-of-magnitude difference between the turnover time and the half-life of 83m Kr of 1.83 h, source atoms have the highest probability to reach the centre of the TPC 13 min after their injection, allowing for a homogeneous distribution before undergoing radioactive decay. We further analyse the thermal aspects of dual-phase operation and define the requirements for the formation of a stable gas pocket on top of the liquid. We find a best-estimate value for the heat transfer rate at the liquid-gas interface of 62 W with an upper limit of 144 W and a minimum gas pocket inlet temperature of 89 K to avoid condensation on the acrylic anode. This study also informs the placement of liquid inlets and outlets in the TPC. The presented techniques are widely applicable to other large-scale, noble-liquid detectors.

47 OTHER INSTRUMENTATION↗

NASA NTRS2005

Modelling the Neutral Atmosphere and Plasma Environment of Saturn

The first year of this contract has resulted in two publications with the P.I. and co-I Jurac as lead authors and two publications where these team members are co-authors. These papers discuss modeling work undertaken in preparation for Cassini; the goal was to summarize our current best knowledge of the ion and neutrals sources and distributions. One of the major goals of this project is to improve models of the plasma and neutral environment near Saturn. The paper "A self-consistent model of plasma and neutrals at Saturn: Neutral cloud morphology" [Jurac and Richardson, 20051 presents results on the neutral clouds near Saturn using a model which for the first times treats the ions and neutrals self-consistently. We also for the first time include a directly sputtered H source. The Voyager and HST observations are used as model constraints. The neutral source is adjusted to give a good match to the HST observations of OH. For this initial run the ion parameters from Richardson et al. are used; charge exchange with ions is a major neutral loss process. The neutral profile derived from the model is then used in a model of plasma transport and chemistry (with the plasma diffusion rate the only free parameter). This model gives new values of the ion composition which are then fed back into the neutral model. This iteration continues until the values converge.

Richardson, John D.↗

DOE OSTI2012

A new extraction system for the Linac4 H{sup -}ion source

As part of the CERN accelerator complex upgrade, a new linear accelerator for H{sup -} (Linac4) is under construction. The ion source design is based on the non-caesiated DESY RF-driven ion source, with the goal of producing an H{sup -} beam of 80 mA beam current, 45 keV beam energy, 0.4 ms pulse length, and 2 Hz repetition rate. The source has been successfully commissioned for an extraction voltage of 35 kV, corresponding to the one used at DESY. Increasing the extraction voltage to 45 kV has resulted in frequent high voltage breakdowns in the extraction region caused by evaporating material from the electron dump, triggering a new design of the extraction and electron dumping system. Results of the ion source commissioning at 35 kV are presented as well as simulations of a new pulsed extraction system for beam extraction at 45 kV.

43 PARTICLE ACCELERATORS↗

DOE OSTI2020

Computational Study of an Iron(II) Polypyridine Electrocatalyst for CO 2 Reduction: Key Roles for Intramolecular Interactions in CO 2 Binding and Proton Transfer

A solar-driven conversion of CO 2 into fuels by artificial photosynthesis would not only mitigate the greenhouse effect but also provide an alternative to obtain fuels in a renewable fashion. To this end, the new iron polypyridine catalyst [Fe(bpy NHEt PY2Me)L 2 ] 2+ (L = H 2 O, CH 3 CN) was recently developed for the electrochemical reduction of CO 2 to CO. Here, we performed density functional theory (DFT) electronic structure calculations to shed light on a possible pathway for CO 2 reduction and the origin of the selectivity between CO 2 reduction versus the hydrogen evolution reaction. The metal center remains Lewis acidic throughout the reduction process due to ligand loss and mainly ligand-based reduction stabilized by antiferromagnetic coupling to a high-spin Fe(II) center. This results in a high barrier for hydride formation but a facile addition and activation of CO 2 via an η 2 coordination and stabilizing hydrogen bonding by the amine group. The second unoccupied equatorial coordination site opens up the possibility for an intramolecular protonation with a coordinated water ligand. This facilitates protonation because not only CO 2 but also the proton source H 2 O is activated and properly aligned for a proton transfer due to the Fe-OH 2 bond; consequently, both protonation steps are facile. The moderate ligand field allows a rapid ligand exchange for a second intramolecular protonation step and facilitates an exergonic CO release. The lower selectivity of the related [Fe(bpy OH PY2Me)L 2 ] 2+ complex can be related to its more acidic second coordination sphere, which enables an intramolecular proton transfer that is kinetically competitive with CO 2 addition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2011

Impedance Measurement of an Antenna with Hydrogen Plasma Driven by 13.56 MHz-rf for J-PARC H{sup -} ion source

In order to satisfy the Japan Proton Accelerator Research Complex (J-PARC) second stage requirements of an H{sup -} ion beam current of 50 mA and a life-time of 2000 hours, the development of a 13.56 MHz-rf-driven H{sup -} ion source was started by using an antenna developed at the Spallation Neutron Source (SNS). As the first step, the impedance of an antenna with hydrogen plasma, which is one of the most important parameters, was measured. For an rf-power of 0 kW, 1.25 kW or 7.45 kW, it was measured as j84.19+5.107 {Omega}, j80.22+11.82 {Omega} or j58.24+21.16 {Omega}, respectively. Its real-part had a rather large value and rather large rf-power dependence unexpectedly. By using the measured impedance, the circuit to produce rf-plasma in the plasma chamber on a -50 kV potential with a 13.56 MHz-rf-source on the ground potential was designed by the circuit simulation code LTSpice IV.

43 PARTICLE ACCELERATORS↗