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At least 145 records · Page 8

Wide-bandgap epitaxial heterojunction windows for silicon solar cells

It is shown that the efficiency of a solar cell can be improved if minority carriers are confined by use of a wide-bandgap heterojunction window. For silicon (lattice constant a = 5.43 A), nearly lattice-matched wide-bandgap materials are ZnS (a = 5.41 A) and GaP (a = 5.45 A). Isotype n-n heterojuntions of both ZnS/Si and GaP/Si were grown on silicon n-p homojunction solar cells. Successful deposition processes used were metalorganic chemical vapor deposition (MO-CVD) for GaP and ZnS, and vacuum evaporation of ZnS. Planar (100) and (111) and texture-etched - (111)-faceted - surfaces were used. A decrease in minority-carrier surface recombination compared to a bare surface was seen from increased short-wavelength spectral response, increased open-circuit voltage, and reduced dark saturation current, with no degradation of the minority carrier diffusion length.

Landis, Geoffrey A.↗

Interface properties of various passivations of HgCdTe

The effects of different surface treatments of the p-type Hg(x-1)Cd(x)Te (x about 0.2) alloy, including anodic-sulfide, anodic-oxide, and ZnS coatings, on the surface charge density and surface mobility were investigated. Measurements of surface recombination velocities in samples passivated by either a ZnS coating on a freshly etched surface or by anodic native sulfide combined with deposited ZnS showed essentially the same temperature dependence down to 50 K. For the same original material, both the surface state density and the activation energy were found to be similar. It is suggested that, for both passivations, the surface is controlled by traps that can be related to lattice defects, such as vacancies.

Schacham, S. E.↗

Large Volume Airborne Contamination Monitoring To Support Nuclear Processes' Deactivation and Decommissioning

Current D and D operations at Hanford have demonstrated a flaw in the current state of the art capability of defining airborne contamination boundaries - Airborne particulate emissions of Pu-239 from CM2H operations on the Hanford Pu Finishing Plant were detected well beyond areas controlled for airborne Pu, putting numerous workers at risk for radiological assimilations - Current air samplers and CAM systems were surveying insufficient volumes of air to accurately predict where respiratory protection was required - Hanford is located in a high radon environment, making air monitoring for alpha emitting actinides challenging in high alpha radon induced backgrounds. - Inexpensive HEPA based home and industrial air purifiers filter significantly higher volumes of air than commercially available continuous-air monitoring (CAM) systems. - Inexpensive models capable of filtered air volumes exceeding 1000 times that of a CAM. - Detector system can be built to detect x-rays generated from actinide decay. - Branching ratios of x-rays are 4 orders of magnitude more intense from Plutonium decay than its gamma emissions. - Detector system can be a low resolution systems, as x-ray region of interest is not terribly congested. - Detection systems evaluated will be designed based on slabs of NaI or pixelated NaI or CsI panels. - Simple graphical user interface software will be developed to operate the detection system. - Concept is to deploy some of these air-purifying systems in nonradiological areas around SRNL to confirm radon can be rejected with confidence. - Generate some filters contaminated with plutonium via electroplated Pu or lab generated simulated particles. - then deploy units in known airborne radiological environments to establish systems ability to accurately measure actinide based hot particles Lab analyses will follow up the system analyses to ensure hot particles were correctly identified. Analysis by Scintillation: - Application of scintillation media to the surface of the filters is being explored. - Evaluating slabs of ZnS(Ag), application of powdered ZnS(Cu) and spray on Perkin Elmer Enhance. - Scintillation events would then be digitized with a digital camera and quantified. - Comparing against sensitivity of a PMT or SiPD readout. - Currently evaluating a Thorlabs 8 Megapixel Monochrome Scientific CCD Camera, hermetically sealed cooled package with a wide angle lens. - Wide angle lens allows complete view of HEPA filter from 7 inches away. - Images taken of glow in the dark paint, as well as plutonium-induced fluorescence. - Plutonium was flamed mounted on a 1 inch diameter stainless steel planchet, covered with a layer of mylar and a section of scintillating ZnS obtained from Eljon. - Currently working on reducing signal-to-noise levels to boost sensitivity. - Dark box to hold contaminated or electroplated source covered filters under fabrication. Analysis by x-ray Spectroscopy: - Branching ratios for x-ray emissions from Plutonium isotopes are orders of magnitude more intense than gamma-ray emissions. - The nuclear databases are incomplete on the branching ratios of some of the isotopes. - Evaluating some custom built SrI2 x-ray spectrometers vs a conventional windowed NaI detector. - SrI2 detectors are carbon-composite-windowed 51 mm x 51 mm. - MCNP calculations to establish self absorbance of filter media on 17 keV x-ray. Radon Rejection: - Activated charcoal pre-filter acts as a Radon trap. - Adding a time lapse feature to camera to aid in radon rejection. SRS Plutonium Fuel Form D and D Operations: Currently deploying air sampler to D and D operation of Pu-238 facility at SRS to generate some field samples to analyze.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Preactivated zeolite nanosheet plate-tiled membrane on porous PVDF film: Synthesis and study of proton-selective ion conduction

Preactivated MFI zeolite nanosheet plates (ZNPs) with large areas (~2.0 × 2.0 μm 2 ) and nanometer thicknesses (~60 nm) were prepared directly in liquid-dispersed state. The individual ZNP was a stack of 4-nm-thick single crystalline zeolite nanosheets (ZNs) interlinked by Si–O–Si bonds between neighboring ZN surfaces. The dispersed open-pore ZNPs allowed formulating suspensions for tiling ZNP membranes on polymer substrates without requiring post-coating activation. A pinhole-free ZNP-tiled (ZNPT) membrane has been achieved on macroporous PVDF film by a self-repairing vacuum-assisted filtration coating method. The resultant ZNPT layer was ~500 nm-thick consisting of about 7 ZNP layers with inter-ZNP width and inter-ZNP entrance porosity around 9 nm and 2%, respectively. The ZNPT-PVDF membrane exhibited high selectivity to proton transport over vanadyl ion and low resistances to proton conduction in aqueous solutions. The membrane also demonstrated to function as an efficient ion separator for the vanadium redox flow battery. The reported synthesis of preactivated ZNP suspension may overcome the major hurdle to realizing polymer-supported ZN membranes, which is the inefficiency of existing methods in obtaining readily dispersible open-pore ZNs. Finally, the ZNPT-PVDF membrane can be a more affordable and sustainable alternative to the Nafion-based ion separation membranes.

36 MATERIALS SCIENCE↗

Simulated Aquifer Heterogeneity Leads to Enhanced Attenuation and Multiple Retention Processes of Zinc

Alluvial aquifers serve as one of the main water sources for domestic, agricultural, and industrial purposes globally. Groundwater quality, however, can be threatened by naturally occurring and anthropogenic metal contaminants. Differing hydrologic and biogeochemical conditions between predominantly coarse-grained aquifer sediments and embedded layers or lenses of fine-grained materials lead to variation in metal behavior. Here, we examine processes controlling Zn partitioning within a dual-pore domain-reconstructed alluvial aquifer. Natural coarse aquifer sediments from the Wind River-Little Wind River floodplain near Riverton, WY, were used in columns with or without fine-grained lenses to examine biogeochemical controls on Zn concentrations, retention mechanisms, and transport. Furthermore, following the introduction of Zn to the groundwater source, Zn preferentially accumulated in the fine-grained lenses, despite their small volumetric contributions. While the clay fraction dominated Zn retention in the sandy aquifer, the lenses supported additional reaction pathways of retention—the reducing conditions within the lenses resulted in ZnS precipitation, overriding the contribution of organic matter. Zinc concentration in the groundwater controlled the formation of Zn-clays and Zn-layered double hydroxides, whereas the extent of sulfide production controlled precipitation of ZnS. Our findings illustrate how both spatial and compositional heterogeneities govern the extent and mechanisms of Zn retention in intricate groundwater systems, with implications for plume behavior and groundwater quality.

54 ENVIRONMENTAL SCIENCES↗

Surface Effects on Pyrene Luminescence Excitation

Pyrene is a polycyclic aromatic hydrocarbon with fluorescence in the 370-400 nm range. The optical properties of pyrene deposited on different substrates were investigated from experimental and theoretical points of view. In contrast to prior studies of surface-enhanced fluorescence, in this work all substrates were semiconductors or insulators. Experimentally, the intensity of photoluminescence (PL) and PL excitation (PLE) spectra were investigated. PLE spectra of pyrene’s monomer emission show that the intensities of the two main absorption peaks vary according to the chosen substrate. Here, calculations for pyrene on zinc sulfide (ZnS) and surface-oxidized diamond suggest that this connection arises from the alignment of the pyrene electronic levels relative to the band edges of the substrate. The absorption peak at 272 nm (4.56 eV) is shown to depend on the HOMO-1→LUMO orbital contribution while the 335 nm (3.70 eV) peak depends upon the HOMO→LUMO transition. When the HOMO-1 level falls inside the substrate valence band, as in the case of ZnS, there is significant hybridization of the molecular state with surface states that causes an enhancement of the 272 nm peak. For pyrene on diamond, however, the HOMO-1 level falls in the substrate bandgap, leading to negligible hybridization and thus no enhancement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Performance of Spherical Quantum Well Down Converters in Solid State Lighting

We report the color conversion performance of amber and red emitting quantum dots (QDs) on InGaN solid-state lighting (SSL) light emitting diode (LED) packages. Spherical quantum well (SQW) architectures (CdS/CdSe 1- x S x /CdS) were prepared using a library of thio- and selenourea synthesis reagents and high throughput synthesis robotics. CdS/CdSe 1- x S x QDs with narrow luminescence bands were coated with thick CdS shells (thickness = 1.6-7.5 nm) to achieve photoluminescence quantum yields (PLQY) up to 88% at amber and red emission wavelengths (λ max = 600-642 nm, FWHM < 45 nm). The photoluminescence from SQWs encapsulated in silicone and deposited on LED packages was monitored under accelerated aging conditions (oven temperature = 85 °C, relative humidity = 5-85%, blue optical power density = 3-45 W/cm 2 ) by monitoring the red photon output over several hundred hours of continuous operation. The growth of a ZnS shell on the SQW surface increases the stability under long-term operation but also reduces the PLQY, especially of SQWs with thick CdS shells. The results illustrate that the outer ZnS shell layer is key to optimizing the PLQY and the long-term stability of QDs during operation on SSL packages.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Elucidating the Discharge Behavior of Aqueous Zinc Sulfur Batteries in the Presence of Molybdenum(IV) Chalcogenide Catalyst: The Criticality of Interfacial Electrochemistry

The aqueous zinc-sulfur battery holds promise for significant capacity and energy density with low cost and safe operation based on environmentally benign materials. However, it suffers from the sluggish kinetics of the conversion reaction. Here, we highlight the efficacy of molybdenum(IV) sulfide (MoS 2 ) to reduce the overpotential of S-ZnS conversion in aqueous electrolytes and study the discharge products formed at the solid-solid and solid-liquid interfaces using experimental and theoretical approaches. Specifically, the MoS 2 -catalyzed electrochemical conversion reaction is characterized via ex situ X-ray diffraction (XRD), transmission electron microscopy (TEM) with energy dispersive spectroscopy (EDS), Raman spectroscopy, synchrotron-based Mo K-edge X-ray absorption spectroscopy (XAS), and in situ synchrotron-based X-ray computed tomography (XCT). Additionally, operando synchrotron-based S K-edge XAS and X-ray fluorescence (XRF) maps are collected to determine the spatial evolution of sulfur-based species at the electrode-electrolyte interface. Further, coupling the operando S K-edge XAS data with the simulated spectra and fitting the data suggested a possible ZnS 2 intermediate phase.

25 ENERGY STORAGE↗

Programmable Phase Selection between Altermagnetic and Noncentrosymmetric Polymorphs of MnTe on InP via Molecular Beam Epitaxy

Phase selecting nearly degenerate crystalline polymorphs during epitaxial growth can be challenging yet critical to targeting physical properties for specific applications. Here, we establish how phase selectivity of altermagnetic and noncentrosymmetric polymorphs of MnTe can be programmed by subtle changes to the surface of lattice-matched InP substrates in molecular beam epitaxy growth. Bulk altermagnetic MnTe is thermodynamically stable in the hexagonal NiAs-structure and is synthesized here on the polar (111)A surface (In-terminated) of InP, while the noncentrosymmetric, cubic ZnS-structure with wide band gap (>3 eV), which epitaxially matches III–V materials, is stabilized on the (111)B surface (P-terminated). Electron microscopy, X-ray photoemission spectroscopy, and reflection high-energy electron diffraction indicate that phase selection is triggered at the interface and proceeds along the growing surface. First-principles calculations suggest that interfacial termination and strain have a significant effect on the interfacial energy; stabilizing the NiAs polymorph on the In-terminated surface and the ZnS structure on the P-terminated surface. Here, selectively grown, high-quality, phase pure films of both MnTe polymorphs will enable our understanding of the novel properties of these materials, thereby facilitating their use in new applications ranging from spintronics to microelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Heteroepitaxial chemistry of zinc chalcogenides on InP nanocrystals for defect-free interfaces with atomic uniformity

Heteroepitaxy on colloidal semiconductor nanocrystals is an essential strategy for manipulating their optoelectronic functionalities. However, their practical synthesis typically leads to scattered and unexpected outcomes due to the intervention of multiple reaction pathways associated with complicated side products of reactants. Here, the heteroepitaxy mechanism of zinc chalcogenide initiated on indium phosphide (InP) colloidal nanocrystals is elucidated using the precursors, zinc carboxylate and trialkylphosphine selenide. The high magnetic receptivity of 77 Se and the characteristic longitudinal optical phonon mode of ZnSe allowed for monitoring the sequence of epilayer formation at the molecular level. The investigation revealed the sterically hindered acyloxytrialkylphosphonium and diacyloxytrialkylphosphorane to be main intermediates in the surface reaction, which retards the metal ion adsorption by a large steric hindrance. The transformation of adsorbates to the crystalline epilayer was disturbed by surface oxides. Raman scattering disclosed the pathway of secondary surface oxidation triggered by carboxylate ligands migrated from zinc carboxylate. The surface-initiated heteroepitaxy protocol is proposed to fabricate core/shell heterostructured nanocrystals with atomic-scale uniformity of epilayers. Despite the large lattice mismatch of ZnS to InP, we realised a uniform and interface defect-free ZnS epilayer (~0.3 nm thickness) on InP nanocrystals, as evidenced by a high photoluminescence quantum yield of 97.3%.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Field-induced partial disorder in a Shastry-Sutherland lattice

Abstract A 2-Q antiferromagnetic order of the ferromagnetic dimers was found below T N = 2.9 K in the Shastry-Sutherland lattice BaNd 2 ZnS 5 by single crystal neutron diffraction. The magnetic order can be understood by the orthogonal arrangement of local Ising Nd spins, identified by polarized neutrons. A field was applied along [1 -1 0] to probe the observed metamagnetic transition in the magnetization measurement. The field decouples two magnetic sublattices corresponding to the propagation vectors q 1 = (½, ½, 0) and q 2 = (−½, ½, 0), respectively. Each sublattice shows a “stripe” order with a Néel-type arrangement in each single layer. The “stripe” order with q 1 remains nearly intact up to 6 T, while the other one with q 2 is suppressed at a critical field H c ~1.7 T, indicating a partial disorder. The H c varies with temperature and is manifested in the H - T phase diagram constructed by measuring the magnetization in BaNd 2 ZnS 5 .

36 MATERIALS SCIENCE↗

Large field-of-view event-mode camera for high-precision epithermal neutron resonance imaging

A large-area event-mode camera system coupled with a 6 LiF-ZnS:Ag scintillator is applied for neutron resonance imaging (NRI) on the energy-resolved neutron imaging (ERNI) flight path, also known as Flight Path 5 (FP5), at the Los Alamos Neutron Science Center (LANSCE). This novel neutron imaging system, featuring a 120 x 120 mm 2 field of view, efficiently captures resonance information across the entire image in a single acquisition, significantly reducing beam time requirements compared to conventional energy-resolved neutron imaging systems. High-quality neutron radiographs with enhanced spatial resolution are achieved through the reconstruction of neutron events based on observations of individual photons emitted from the scintillator. The system demonstrates reduced background through neutron/gamma discrimination capabilities while maintaining sharpness across a large fields of view. In the measurements presented here, a spatial resolution of approximately 340 μm was achieved using center-of-gravity photon cluster centroiding. We demonstrate the system’s capability for quantitatively determining isotopic distributions in various thin samples, as well as automatically reconstructing complex scenes with overlapping resonances from diverse samples. These results are obtained using standard data analysis tools, despite the relatively slow 6 LiF-ZnS:Ag scintillator, which may not be optimal for absorption resonance detection. The capabilities demonstrated here offer a valuable, versatile, and cost-effective solution for high spatial and temporal resolution, large field-of-view energy-resolved neutron imaging, with potential applications across various scientific and industrial domains.

36 MATERIALS SCIENCE↗

Scintillator-based Timepix3 detector for neutron spin-echo techniques using intensity modulation

A scintillator-based Timepix3 (TPX3) detector was developed to resolve the high-frequency modulation of a neutron beam in both spatial and temporal domains, as required for neutron spin-echo experiments. In this system, light from a scintillator is manipulated with an optical lens and is intensified using an image intensifier, making it detectable with the TPX3 chip. Two different scintillators, namely, 6 LiF:ZnS(Ag) and 6 LiI:Eu, were investigated to achieve the high resolution needed for spin-echo modulated small-angle neutron scattering (SEMSANS) and modulation of intensity with zero effort (MIEZE). The methodology for conducting event-mode analysis is described, including the optimization of clustering parameters for both scintillators. The detector with both scintillators was characterized with respect to detection efficiency, spatial resolution, count rate, uniformity, and γ-sensitivity. The 6 LiF:ZnS(Ag) scintillator-based detector achieved a spatial resolution of 200 μm and a count rate capability of 1.1 × 10 5 cps, while the 6 LiI:Eu scintillator-based detector demonstrated a spatial resolution of 250 μm and a count rate capability exceeding 2.9 × 10 5 cps. Furthermore, high-frequency intensity modulations in both spatial and temporal domains were successfully observed, confirming the suitability of this detector for SEMSANS and MIEZE techniques, respectively.

47 OTHER INSTRUMENTATION↗

Longwave infrared (6.6–11.4 µm) dual-comb spectroscopy with 240,000 comb-mode-resolved data points at video rate

Using sub-3-cycle pulses from mode-locked Cr:ZnS lasers at λ ≈ 2.4 µm as a driving source, we performed high-resolution dual-frequency-comb spectroscopy in the longwave infrared (LWIR) range. A duo of highly coherent broadband (6.6–11.4 µm) frequency combs were produced via intrapulse difference frequency generation in zinc germanium phosphide (ZGP) crystals. Fast (up to 0.1 s per spectrum) acquisition of 240,000 comb-mode-resolved data points, spaced by 80 MHz and referenced to a Rb clock, was demonstrated, resulting in metrology grade molecular spectra of N 2 O (nitrous oxide) and CH 3 OH (methane). The key to high-speed massive spectral data acquisition was low intensity and phase noise of the LWIR combs and high (7.5%) downconversion efficiency, resulting in a LWIR power of 300 mW for each comb.

Vasilyev, Sergey (ORCID:0000000225203547)↗

Drift in interference filters. II - Radiation effects

Studies of peak transmission drift in narrow-band interference filters have shown that there exist two mechanisms that cause drift toward shorter wavelengths. One is dependent on the thermal history of the filter and is discussed in Part 1 of this paper. The other is dependent on the exposure of the filter to radiation. For ZnS-cryolite filters of particular design, it is experimentally demonstrated that the filters are most sensitive to radiation in a 100-A band centered at approximately 3900 A. The drift rate in the focal plane of an f/20 solar image is approximately 3 A/100 hr of exposure. Further, it is also shown by model calculations that the observed radiation-induced drift is consistent with the hypothesis that the optical thickness of ZnS decreases in proportion to the radiant energy absorbed.

Title, A. M.↗

Deposition and characterization of ZnS/Si heterojunctions produced by vacuum evaporation

Isotype heterojunctions of ZnS (lattice constant 5.41 A) were grown on silicon (lattice constant 5.43 A) p-n junctions to form a minority-carrier mirror. The deposition process was vacuum evaporation from a ZnS powder source onto a heated (450 C) substrate. Both planar (100) and textured (111) surfaces were used. A reduction of the minority-carrier recombination at the surface was seen from increased short-wavelength quantum response and increased illuminated open-circuit voltage. The minority-carrier diffusion length was not degraded by the process.

Landis, Geoffrey A.↗

Electroluminescent Displays Made With Alternative Dopants

Metals and metal fluorides deposited in ZnS to form color phosphors. Single-layer, thin-film electroluminescent display device contains ZnS host layer doped to form green, red, and blue phosphors. Luminescence in chosen colors at chosen intersections between rows and columns produced by application of voltages to appropriate row-and-column pairs of conductors.

Robertson, James B.↗

Design of a Three-Layer Antireflection Coating for High Efficiency Indium Phosphide Solar Cells Using a Chemical Oxide as First Layer

It is well known that the behavior of III-V compound based solar cells is largely controlled by their surface, since the majority of light generated carriers (63% for GaAs and 79% for InP) are created within 0.2 microns of the illuminated surface of the cell. Consequently, the always observed high surface recombination velocity (SRV) on these cells is a serious limiting factor for their high efficiency performance, especially for those with the p-n junction made by either thermal diffusion or ion implantation. A good surface passivation layer, ideally, a grown oxide as opposed to a deposited one, will cause a significant reduction in the SRV without adding interface problems, thus improving the performance of III-V compound based solar cells. Another significant benefit to the overall performance of the solar cells can be achieved by a substantial reduction of their large surface optical reflection by the use of a well designed antireflection (AR) coating. In this paper, we demonstrate the effectiveness of using a chemically grown, thermally and chemically stable oxide, not only for surface passivation but also as an integral part of a 3- layer AR coating for thermally diffused p(+)n InP solar cells. A phosphorus-rich interfacial oxide, In(PO3)3, is grown at the surface of the p(+) emitter using an etchant based on HNO3, o-H3PO4 and H2O2. This oxide has the unique properties of passivating the surface as well as serving as a fairly efficient antireflective layer yielding a measured record high AM0, 25 C, open-circuit voltage of 890.3 mV on a thermally diffused InP(Cd,S) solar cell. Unlike conventional single layer AR coatings such as ZnS, Sb2O3, SiO or double layer AR coatings such as ZnS/MgF2 deposited by e-beam or resistive evaporation, this oxide preserves the stoichiometry of the InP surface. We show that it is possible to design a three-layer AR coating for a thermally diffused InP solar cell using the In(PO3)3 grown oxide as the first layer and Al2O3, MgF2 or ZnS, MgF2 as the second and third layers respectively, so as to yield an overall theoretical reflectance of less than 2%. Since chemical oxides are readily grown on III-V semiconductor materials, the technique of using the grown oxide layer to both passivate the surface as well as serve as the first of a multilayer AR coating, should work well for essentially all III-V compound-based solar cells.

Moulot, Jacques↗