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At least 487 records · Page 27

Fabrication of advanced accident tolerant U-Si fuel forms

Prospective advanced accident tolerant UN-USi fuel forms for light-water reactors are being studied at Los Alamos National Laboratory. In this paper we present a recent effort to fabricate and characterize U{sub 3}Si{sub 5} and UN-U{sub 3}Si{sub 5} fuel. The U{sub 3}Si{sub 5} is prepared by arc-melting stoichiometric amounts of uranium and silicon metals. The arc melting process consists of cutting U metal plate into small pieces that can be placed in a tri-arc furnace for melting. The material is slowly heated until a uniform melt of the U and Si is achieved. The fabrication of the U{sub 3}Si{sub 5} pellets followed a conventional cold-press and sinter process. As for the fabrication of UN-U{sub 3}Si{sub 5}, the uranium nitride (UN) feedstock powder was synthesized using carbothermic reduction nitridation. The UN is milled and sieved to sub-74 μm. The UN was mixed with EBS (ethylene bis-stearamide) and milled for 45 minutes. The UN-EBS was combined with 10 wt.% U{sub 3}Si{sub 5} powder (equivalent to 15 vol.% in UN) and additional EBS. The fabrication of the UN-U{sub 3}Si{sub 5} pellets followed a conventional cold-press and sinter process similar to that used to fabricate the U{sub 3}Si{sub 5} pellets. A sample UN-U{sub 3}Si{sub 5} pellet was cross-sectioned, ground, and polished for optical microscopy. The UN and U{sub 3}Si{sub 5} phases are apparent as well as pores and micro-cracks. The affect of micro-cracking on fuel performance is unknown and should be assessed during post-irradiation examination.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Non-resonant Bragg scattering four-wave mixing at near-visible wavelengths in low-confinement silicon nitride waveguides

Quantum state coherent frequency conversion processes—such as Bragg-scattering four-wave mixing (BSFWM)—hold promise as a flexible technique for networking heterogeneous and distant quantum systems. In this Letter, we demonstrate BSFWM within an extended (1.2-m) low-confinement silicon nitride waveguide and show that this system has the potential for near-unity frequency conversion in visible and near-visible wavelength ranges. Using sensitive classical heterodyne laser spectroscopy at low optical powers, we characterize the Kerr coefficient (∼1.55 W −1 m −1 ) and linear propagation loss (∼0.0175 dB/cm) of this non-resonant waveguide system, revealing a record-high nonlinear figure of merit (NFM = γ / α ≈ 3.85 W −1 ) for BSFWM of near-visible light in non-resonant silicon nitride waveguides. We predict how, at high yet achievable on-chip optical powers, this NFM would yield a comparatively large frequency conversion efficiency, opening the door to near-unity flexible frequency conversion without cavity enhancement and resulting bandwidth constraints.

Jaber, Nicholas (ORCID:000900070106809X)↗

Charge Recombination, Transport Dynamics, and Interfacial Effects in Organic Solar Cells

The need for renewable sources of energy is well known. Conversion of sunlight to electricity using solar cells is one of the most important opportunities for creating renewable energy sources. The research carried out under DE-FG02-08ER46535 focused on the science and technology of “Plastic” solar cells comprised of organic (i.e. carbon based) semiconductors. The Bulk Heterojunction concept involves a phase separated blend of two organic semiconductors each with dimensions in the nano-meter length scale --- one a material that functions as a donor for electrons and the other a material that functions as an acceptor for electrons. The nano-scale inter-penetrating network concept for “Plastic” solar cells was created at UC Santa Barbara. A simple measure of the impact of this concept can be obtained from a Google search which gives 244,000 “hits” for the Bulk Heterojunction solar cell. Research funded through this program focused on four major areas: 1. Interfacial effects in organic photovoltaics, 2. Charge transfer and photogeneration of mobile charge carriers in organic photovoltaics, 3. Transport and recombination of the photogenerated charge carriers in organic photovoltaics, 4. Synthesis of novel organic semiconducting polymers and semiconducting small molecules, including conjugated polyelectrolytes. Following the discovery of ultrafast charge transfer at UC Santa Barbara in 1992, the nano-organic (Bulk Heterojunction) concept was formulated. The need for a morphology comprising two interpenetrating bicontinuous networks was clear: one network to carry the photogenerated electrons (negative charge) to the cathode and one network to carry the photo-generated holes (positive charge) to the anode. This remarkable self-assembled network morphology has now been established using Transmission electron Microscopy (TEM) either in the Phase Contrast mode or via TEM-Tomography. The steps involved in delivering power from a solar cell to an external circuit are the following: • Photo-excitation of the donor (or the acceptor). • Charge transfer with holes in the donor domain and electrons in the acceptor domain. • Sweep-out to electrodes prior to recombination by the internal electric field. • Energy delivered to the external circuit. Each of these four steps was studied in detail using a wide variety of organic semiconductors with different molecular structures. This UC Santa Barbara group was the first to clarify the origin and the mechanism involved in the ultrafast charge transfer process. The ultrafast charge transfer (time scale approximately 100 times faster than the first step in the photo-synthesis of green plants) is the fundamental reason for the potential for high power conversion efficiency of sunlight to electricity from plastic solar cells. The UCSB group was the first to emphasize, clarify and demonstrate the need for sweep-out to electrodes prior to recombination by the internal electric field. The UCSB group was the first to synthesize small molecule organic semiconductors capable of high power conversion efficiencies. The results of this research were published in high impact peer-reviewed journals. Our published papers (40 in number) provide answers to fundamental questions that have been heavily discussed and debated in the field of Bulk Heterojunction Solar Cells; scientific questions that must be resolved before this technology can be ready for commercialization in large scale for production of renewable energy. Of the forty publications listed, nineteen were co-authored by two or more of the PIs, consistent with the multi-investigator approach described in the original proposal. The specific advantages of this “plastic” solar cell technology are the following: a. Manufacturing by low-cost printing technology using soluble organic semiconductors; this approach can be implemented in large scale by roll-to-roll printing on plastic substrates. b. Low energy cost in manufacturing; all steps carried out at room temperature (approx. a factor of ten less than the use of Silicon which requires high temperature processing). c. Low carbon footprint d. Lightweight, flexible and rugged Because of the resolution of many scientific issues, a significant fraction of which were addressed in the research results of DE-FG02-08ER46535, the power conversion efficiencies are improving at an ever increasing rate. During the funding period of DE-FG02-08ER46535, the power conversion efficiencies of plastic solar cells improved from just a few per cent to values greater than 11% with contributions from our group and from researchers all over the world.

14 SOLAR ENERGY↗

Flash (Ultra-Rapid) Spark-Plasma Sintering of Silicon Carbide

A new ultra-rapid process of flash spark plasma sintering is developed. The idea of flash spark plasma sintering (or flash hot pressing - FHP) stems from the conducted theoretical analysis of the role of thermal runaway phenomena for material processing by flash sintering. The major purpose of the present study is to theoretically analyze the thermal runaway nature of flash sintering and to experimentally address the challenge of uncontrollable thermal conditions by the stabilization of the flash sintering process through the application of the external pressure. The effectiveness of the developed FHP technique is demonstrated by the few seconds–long consolidation of SiC powder in an industrial spark plasma sintering device. Specially designed sacrificial dies heat the pre-compacted SiC powder specimens to a critical temperature before applying any voltage to the powder volume and allowing the electrode-punches of the SPS device setup to contact the specimens and pass electric current through them under elevated temperatures. The experimental results demonstrate that flash sintering phenomena can be realized using conventional SPS devices. The usage of hybrid heating SPS devices is pointed out as the mainstream direction for the future studies and utilization of the new flash hot pressing (ultra-rapid spark plasma sintering) technique.

36 MATERIALS SCIENCE↗

Characterization of thin film deposits on tungsten filaments in catalytic chemical vapor deposition using 1,1-dimethylsilacyclobutane

Metal filament plays a key role in the technique of catalytic chemical vapor deposition (Cat-CVD) as it serves as a catalyst in dissociating the source gas to form reactive species. These reactive species initiate the gas-phase reaction chemistry and final thin film and nanostructure formation. At the same time, they also react with the metal itself, leading to the formation of metal alloys and other deposits. The deposits on the tungsten filaments when exposed to 1,1-dimethylsilacyclobutane (DMSCB), a single-source precursor for silicon carbide thin films, in the process of Cat-CVD were studied in this work. It has been demonstrated that a rich variety of deposits, including tungsten carbides (W{sub 2}C and WC), tungsten silicide (W{sub 5}Si{sub 3}), silicon carbide, amorphous carbon, and graphite, form on the W filament surfaces. The structural and morphological changes in the tungsten filaments depend strongly on the DMSCB pressure and filament temperature. At 1000 and 2000 °C, the formation of WC and W{sub 2}C dominates. In addition, a thin amorphous carbon layer has been found at 1500 °C with the 0.12 and 0.24 Torr of DMSCB and a lower temperature of 1200 °C with the 0.48 Torr of DMSCB. An increase in the DMSCB sample pressure gives rise to higher Si and C contents. As a result, the formation of SiC and W{sub 5}Si{sub 3} has been observed with the two high-pressure DMSCB samples (i.e., 0.24 and 0.48 Torr). The rich decomposition chemistry of DMSCB on the W surfaces is responsible for the extensive changes in the structure of the W filament, providing support for the close relationship between the gas-phase decomposition chemistry and the nature of alloy formation on the metal surface. The understanding of the structural changes obtained from this work will help guide the development of efficient methods to solve the filament aging problem in Cat-CVD and also to achieve a controllable deposition process.

36 MATERIALS SCIENCE↗

Light emission from silicon nanocrystals

The main experimental results of studies of the photoluminescence of silicon nanocrystals and theoretical methods developed for the description of optical processes occurring in them are reviewed. Special attention is focused on silicon nanocrystals in the SiO{sub 2} matrix that were the object of most of the studies. Two fundamental theoretical methods described in detail are the multiband effective-mass method and the tight-binding method which have found wide application in simulating various processes occurring in nanostructures. A phenomenological model for excitons self-trapped on the surface of oxidized silicon nanocrystals, which has been recently developed on the basis of experimental results obtained by femtosecond spectroscopy, is reported.

36 MATERIALS SCIENCE↗

Fabrication of nanostructured silicon surface using selective chemical etching

A two-stage process based on selective chemical etching induced by metal nanoclusters is used to fabricate nanostructured surfaces of silicon plates with a relatively low reflectance. At silicon surfaces covered with silver nanoclusters, the SERS effect is observed for rhodamine concentrations of about 10{sup –12} M. At certain technological parameters, the depth of the nanostructured layer weakly depends on the conditions for the two-stage etching, in particular, etching time. Under otherwise equal conditions for etching, the rate of the formation of textured layer in the p-type silicon is two times greater than the formation rate in the n-type silicon.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Reducing the Cost of Solar Cells

Solar-powered electricity prices could soon approach those of power from coal or natural gas thanks to collaborative research with solar startup Ampulse Corporation at the National Renewable Energy Laboratory. Silicon wafers account for almost half the cost of today's solar photovoltaic panels, so reducing or eliminating wafer costs is essential to bringing prices down. Current crystalline silicon technology converts energy in a highly efficient manner; however, that technology is manufactured with processes that could stand some improvement. The industry needs a method that is less complex, creates less waste and uses less energy. First, half the refined silicon is lost as dust in the wafer-sawing process, driving module costs higher. Wafers are sawn off of large cylindrical ingots, or boules, of silicon. A typical 2-meter boule loses as many as 6,000 potential wafers during sawing. Second, the wafers produced are much thicker than necessary. To efficiently convert sunlight into electricity, the wafers need be only one-tenth the typical thickness. NREL, the Oak Ridge National Laboratory and Ampulse have partnered on an approach to eliminate this waste and dramatically lower the cost of the finished solar panels. By using a chemical vapor deposition process to grow the silicon on inexpensive foil, Ampulse is able to make the solar cells just thick enough to convert most of the solar energy into electricity. No more sawdust - and no more wasting refined silicon materials. NREL developed the technology to grow high-quality silicon and ORNL developed the metal foil that has the correct crystal structure to support that growth. Ampulse is installing a pilot manufacturing line in NREL's Process Development Integration Laboratory, where solar companies can work closely with lab scientists on integrated equipment to answer pressing questions related to their technology development, as well as rapidly overcoming R and D challenges and risk. NREL's program is focused on transformative innovation in the domestic PV industry. With knowledge and expertise acquired from the PDIL pilot production line tools, Ampulse plans to design a full-scale production line to accommodate long rolls of metal foil. The Ampulse process 'goes straight from pure silicon-containing gas to high-quality crystal silicon film,' said Brent Nelson, the operational manager for the Process Development Integration Laboratory. 'The advantage is you can make the wafer just as thin as you need it - 10 microns or less.' Most of today's solar cells are made out of wafer crystalline silicon, though thin-film cells made of more exotic elements such as copper, indium, gallium, arsenic, cadmium, tellurium and others are making a strong push into the market. The advantage of silicon is its abundance, because it is derived from sand. Silicon's disadvantage is that purifying it into wafers suitable for solar cells can be expensive and energy intensive. Manufacturers add carbon and heat to sand to produce metallurgical-grade silicon, which is useful in other industries, but not yet suitable for making solar cells. So this metallurgical-grade silicon is then converted to pure trichlorosilane (SiCl3) or silane (SiH4) gas. Typically, the purified gas is then converted to create a silicon feedstock at 1,000 degrees Celsius. This feedstock is melted at 1,414 C and recrystallized into crystal ingots that are finally sawed into wafers. The Ampulse method differs in that it eliminates the last two steps in the traditional process and works directly with the silane gas growing only the needed silicon right onto a foil substrate. A team of NREL scientists had developed a way to use a process called hot-wire chemical vapor deposition to thicken silicon wafers with near perfect crystal structure. Using a hot tungsten filament much like the one found in an incandescent light bulb, the silane gas molecules are broken apart and deposited onto the wafer using the chemical vapor deposition technique at about 700 C - a much lower temperature than needed to make the wafer. The hot filament decomposes the gas, allowing silicon layers to deposit directly onto the substrate. Armed with this new technique, Branz and Teplin searched for ways to grow the silicon on cheaper materials and still use it for solar cells. They found the ideal synergy when visiting venture capitalists from Battelle Ventures asked them whether they could do anything useful with a breakthrough from Oak Ridge's superconducting wire development group. The new development, called the rolling assisted biaxially textured substrate (RABiTS), was just the opportunity the two scientists had been seeking. If metal foil is to work as a substrate, it must be able to act as a seed crystal so the silicon can grow on it with the correct structure. The RABiTS process forms crystals in the foil that are correctly oriented to receive the silicon atoms and lock them into just the right positions.

14 SOLAR ENERGY↗

Effect of Barothermal Processing on the Solid-State Formation of the Structure and Properties of 16 at % Si–Al Hypereutectic Alloy

We describe barothermal processing (hot isostatic pressing) of a 16 at % Si–Al binary alloy for 3 h at a temperature of 560°C and pressure of 100 MPa for 3 h, in combination with measurements of heat effects during cooling. The results demonstrate that this processing leads to the fragmentation of the silicon structural constituent and ensures a high degree of homogenization of the as-prepared alloy. Heat treatment of the 16 at % Si–Al alloy at 560°C and a pressure of 100 MPa leads to a thermodynamically driven enhanced silicon dissolution, up to ~10 at %, in the aluminum matrix, resulting in the formation of a supersaturated solid solution, which subsequently decomposes during cooling. We analyze the complete porosity elimination process, which makes it possible to obtain a material with 100% relative density. According to differential barothermal analysis, microstructural analysis, and scanning and transmission electron microscopy data, barothermal processing of the 16 at % Si–Al alloy produces a bimodal size distribution of the silicon phase constituent: microparticles 3.6 μm in average size and nanoparticles down to ~1 nm in diameter. The Al matrix has been shown to contain a high density of edge dislocations. Barothermal processing reduces the thermal expansion coefficient and microhardness of the hypereutectic alloy. We conclude that solid-state barothermal processing is an effective tool for completely eliminating microporosity from the 16 at % Si–Al alloy, reaching a high degree of homogenization, and controlling the microstructure of the alloy, in particular by producing high dislocation density in the aluminum matrix.

36 MATERIALS SCIENCE↗

CORRELATED STRONTIUM AND BARIUM ISOTOPIC COMPOSITIONS OF ACID-CLEANED SINGLE MAINSTREAM SILICON CARBIDES FROM MURCHISON

We present strontium, barium, carbon, and silicon isotopic compositions of 61 acid-cleaned presolar SiC grains from Murchison. Comparison with previous data shows that acid washing is highly effective in removing both strontium and barium contamination. For the first time, by using correlated {sup 88}Sr/{sup 86}Sr and {sup 138}Ba/{sup 136}Ba ratios in mainstream SiC grains, we are able to resolve the effect of {sup 13}C concentration from that of {sup 13}C-pocket mass on s-process nucleosynthesis, which points toward the existence of large {sup 13}C pockets with low {sup 13}C concentrations in asymptotic giant branch stars. The presence of such large {sup 13}C pockets with a variety of relatively low {sup 13}C concentrations seems to require multiple mixing processes in parent asymptotic giant branch stars of mainstream SiC grains.

79 ASTRONOMY AND ASTROPHYSICS↗

Preparation of Nano-SiO{sub 2}-Coated Graphite Films by a Laser-Assisted Sol–Gel Process

Here, we prepared nano-SiO{sub 2}-coated graphite films using a novel laser-assisted sol–gel method. The SiO{sub 2} sol–gel prepositioned on the graphite substrate was irradiated by the fiber laser at different energy densities. The growth mechanism of the coatings under laser irradiation was studied and the effects of processing parameters on the coating structure were systematically investigated. In addition, the high-temperature oxidation resistance of these samples was examined. Surface morphology and elemental composition were examined using scanning electron microscopy and energy-dispersive spectrometer. Phase constituents and microstructure were identified by x-ray diffraction and transmission electron microscopy. The oxidation resistance was analyzed by thermal gravimetric analysis. The results found that laser irradiation significantly modifies the sol–gel-deposited nano-SiO{sub 2} layer. A uniform and compact nano-SiO{sub 2} coating was obtained when irradiated by laser energy density of 14.4 kJ/cm{sup 2}. Optimum high-temperature oxidation resistance was achieved for the two-layer SiO{sub 2}-coated films.

36 MATERIALS SCIENCE↗

Electro-Optic Modulation Using Metal-Free Perovskites

Electro-optic (EO) modulation is of interest to impart information onto an optical carrier. Inorganic crystals—most notably LiNbO 3 and BaTiO 3 —exhibit EO modulation and good stability, but are difficult to integrate with silicon photonic technology. Solution-processed organic EO materials are readily integrated but suffer from thermal degradation at the temperatures required in operating conditions for accelerated reliability studies. Hybrid organic–inorganic metal halide perovskites have the potential to overcome these limitations; however, these have so far relied on heavy metals such as lead and cadmium. Here, we report linear EO modulation using metal-free perovskites, which maintain the crystalline features of the inorganic EO materials and incorporate the flexible functionality of organic EO chromophores. We find that, by introducing a deficiency of cations, we reduce the symmetry in the perovskite crystal and produce thereby an increased EO response. The best-engineered perovskites reported herein showcase an EO coefficient of 14 pm V –1 at a modulation frequency of 80 kHz, an order of magnitude higher than in the nondefective materials. Furthermore, we observe split peaks in the X-ray diffraction and neutron diffraction patterns of the defective sample, indicating that the crystalline structure has been distorted and the symmetry reduced. Density functional theory (DFT) studies link this decreased symmetry to NH 4 + deficiencies. This demonstration of EO from metal-free perovskites highlights their potential in next-generation optical information transmission.

36 MATERIALS SCIENCE↗

Polystyrene-block-Polydimethylsiloxane as a Potential Silica Substitute for Polysiloxane Reinforcement

We report here on microphase-separated poly(styrene-block-dimethylsiloxane) (PS-b-PDMS) as a reinforcing filler in PDMS thermosets that overcomes the long-standing problem of aging in the processing of silica-reinforced silicone. Surprisingly, PS-b-PDMS reinforced composites display comparable mechanical performance to silica-modified analogs, even though the modulus of PS is much smaller than that of silica and there is no evidence of percolation with respect to the rigid PS domains. We have found that a few unique characteristics contribute to the reinforcing performance of PS-b-PDMS. The strong self-assembly behavior promotes batch-to-batch repeatability by having well-dispersed fillers. The structure and size of the fillers depend on the loading and characteristics of both filler and matrix, along with the shear effect. The reinforcing effect of PS-b-PDMS is mostly brought by the entanglements between the corona layer of the filler and the matrix, rather than the hydrodynamic reinforcement of the PS phase.

36 MATERIALS SCIENCE↗

Nanowire photonic crystal waveguides for single-atom trapping and strong light-matter interactions

We present a comprehensive study of dispersion-engineered nanowire photonic crystal waveguides suitable for experiments in quantum optics and atomic physics with optically trapped atoms. Detailed design methodology and specifications are provided, as are the processing steps used to create silicon nitride waveguides of low optical loss in the near-IR. Measurements of the waveguide optical properties and power-handling capability are also presented.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Characterization of contaminants in the Lyman-alpha forest auto-correlation with DESI

Baryon Acoustic Oscillations can be measured with sub-percent precision above redshift two with the Lyman-α (Lyα) forest auto-correlation and its cross-correlation with quasar positions. This is one of the key goals of the Dark Energy Spectroscopic Instrument (DESI) which started its main survey in May 2021. We present in this paper a study of the contaminants to the Lyα forest which are mainly caused by correlated signals introduced by the spectroscopic data processing pipeline as well as astrophysical contaminants due to foreground absorption in the intergalactic medium. Notably, an excess signal caused by the sky background subtraction noise is present in the Lyα auto-correlation in the first line-of-sight separation bin. We use synthetic data to isolate this contribution, we also characterize the effect of spectro-photometric calibration noise, and propose a simple model to account for both effects in the analysis of the Lyα forest. We then measure the auto-correlation of the quasar flux transmission fraction of low redshift quasars, where there is no Lyα forest absorption but only its contaminants. We demonstrate that we can interpret the data with a two-component model: data processing noise and triply ionized Silicon and Carbon auto-correlations. This result can be used to improve the modeling of the Lyα auto-correlation function measured with DESI.

79 ASTRONOMY AND ASTROPHYSICS↗

Gain characterization of LGAD sensors with beta particles and 28-MeV protons

Low Gain Avalanche Diodes, also known as LGADs, are widely considered for fast-timing applications in high energy physics, nuclear physics, space science, medical imaging, and precision measurements of rare processes. Such devices are silicon-based and feature an intrinsic gain due to a p + -doped layer that allows the production of a controlled avalanche of carriers, with multiplication on the order of 10–100. This technology can provide time resolution on the order of 20–30 ps, and variants of this technology can provide precision tracking too. The characterization of LGAD performance has so far primarily been focused on the interaction of minimum ionizing particles for high energy and nuclear physics applications. This article expands the study of LGAD performance to highly-ionizing particles, such as 28-MeV protons, which are relevant for several future scientific applications, e.g. in biology and medical physics, among others. These studies were performed with a beam of 28-MeV protons from a tandem Van de Graaff accelerator at Brookhaven National Laboratory and beta particles from a ^90Sr source; these were used to characterize the response and the gain of an LGAD as a function of bias voltage and collected charge. Here, the experimental results are also compared to TCAD simulations.

47 OTHER INSTRUMENTATION↗

Operation and performance of the ATLAS silicon micro-strip tracker

The Semiconductor Tracker (SCT) is the key precision tracking device in ATLAS, made from silicon micro-strip detectors processed in the planar p-in-n technology. The completed SCT has been installed inside the ATLAS experimental hall since 2007 and has been operational since then. In this paper the current status of the Semiconductor Tracker is reviewed, including results from the data-taking periods in 2009 and 2010, and from the detector alignment. The emphasis is given to the performance of the Semiconductor Tracker with the LHC in collision mode and to the performance of individual electronic components. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗