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At least 739 records · Page 41

Real-Time Detection of Hydrogen and Ammonia Isotopologues for Impurity Removal and Recovery of Tritium

To accommodate gas measurements for impurity removal and recovery of tritium, a silver-coated optical or waveguide is employed for collecting Raman scattered signals to determine relative hydrogen and ammonia isotopologue populations in real time. The data and results presented here demonstrate an analytical methodology for the analysis of four ammonia and three hydrogen isotopologues in a hydrogen–deuterium exchange reaction by gas phase Raman spectroscopy. Standard chemometric modeling techniques effectively unravel the signatures of the isotopologues involved observed here; however, a sophisticated quantum chemical approach supports the spectral assignments. An interpretation of the data presented here can emphasize the practicality and reliability of the gaseous monitoring system in complex chemical environments for the hydrogen fuel economy as well as the more distant energy source from a facility that handles tritium. There are still considerable concerns about the measurement of tritium in isotope separation and radiological impurities from gas processing. A common impurity in gas processing is ammonia, which can form readily in the presence of nitrogen and tritium. Substituted ammonia (NQ 3 ), where Q = H, D, or T, is traditionally removed through getters or diffusers along with other non-hydrogen contaminants. A preferable analytical approach is noninvasive and can be deployed for real-time process evaluation in radiological environments.

Ammonia↗

Effects of temperature and near-substrate plasma density on the structural and electrical properties of dc sputtered germanium thin films

Germanium thin films were deposited by dc reactive magnetron sputtering as a function of substrate temperature and ion flux using an unbalanced magnetron with an external magnetic field. The ion flux and energy distribution were measured using a retarding field energy analyzer (RFEA), a flat probe with a guard ring, and cylindrical Langmuir probes. The RFEA ion flux, the flat probe saturation currents, and the ion densities inferred from the cylindrical probe data are in very good agreement over a wide range of plasma densities, which were varied both by the external coil current and discharge power. The RFEA ion energy distributions are in good agreement with the plasma potentials inferred from the cylindrical probes, and suggest that the nonuniformity of the plasma in the vicinity of the substrate holder should be considered in the interpretation of probe results in these systems. The deposited films were characterized by x-ray diffraction, Raman spectroscopy, optical transmission, resistivity, and Hall effect measurements. Under low ion bombardment conditions, an abrupt onset of the crystalline phase with respect to temperature is observed in the Raman and x-ray diffraction measurements, and the crystal quality increases with increasing temperature above the transition temperature. The transition is also accompanied by a sharp decrease in film resistivity. The microcrystalline films have a strong preferential orientation in the (220) direction, and are p type with carrier densities in the range 10{sup 18} cm{sup -3} and mobilities in the range 15-30 cm{sup 2}/V-s. The structural and electronic properties of the films are sensitive to the ion flux. Near the transition temperature the effects of increasing ion flux can be attributed to the small temperature rise that accompanies the higher plasma density. At higher temperatures the increased ion flux results in a more random crystallographic orientation, with significantly lower carrier concentrations and only slightly lower carrier mobilities, implying either a reduction in acceptor defect density and/or the creation of compensating n-type defects.

36 MATERIALS SCIENCE↗

Optical characterizations of doped silicon nanocrystals grown by co-implantation of Si and dopants in SiO₂

Co-implantation, with overlapping implantation projected ranges, of Si and doping species (P, As, and B) followed by a thermal annealing step is a viable route to form doped Si nanocrystals (NCs) embedded in silica (SiO₂). In this paper, we investigate optical characterizations of both doped and un-doped Si-NCs prepared by this method. The effective NC presence in the oxide layer and their crystallinity is verified by Raman spectrometry. Photoluminescence (PL) and PL excitation measurements reveal quantum confinement effects and a gradual PL quenching with increasing dopant concentrations. In un-doped NC, the measured Stokes shift remains constant and its value ~0.2 eV is almost twice the Si–O vibration energy. This suggests that a possible radiative recombination path is a fundamental transition assisted by a local phonon. PL lifetime investigations show that PL time-decays follow a stretched exponential. Using a statistical model for luminescence quenching, a typical NC diameter close to 2 nm is obtained for As- and P-doped samples, consistent with our previous atomic probe tomography (APT) analyses. APT also demonstrated that n-type dopant (P and As) are efficiently introduced in the NC core, whereas p-type dopant (B) are located at the NC/SiO₂ interface. This last observation could explain the failure of the luminescence-quenching model to determine NC size in B-doped samples. All together, these experimental observations question on possible different carrier recombination paths in P or As doped NC compared to B one's.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strongly enhanced Raman scattering of graphene by a single gold nanorod

Individual gold nanorods (AuNRs) and monolayer graphene hybrid system is investigated experimentally. Surface enhanced Raman scattering (SERS) signal of the graphene is observed due to a single AuNR with enhancement factor up to ∼1000-fold. The SERS intensity is strongly polarization dependent and the enhancement effect varies with the detuning between the excitation laser and the AuNR resonance. The SERS effect is highest when the resonant wavelength of the AuNRs matches well with the excitation light. By correlating the scattering and photoluminescence, it is demonstrated that the conventional background in SERS ascribes to the photon emission of metallic nanostructures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Three-wave coupling in electron-positron-ion plasmas

The three-wave coupling processes in electron-positron-ion plasmas are investigated. The non-linear dispersion relation is derived along with the non-linear growth rate in both resonant and non resonant processes. It is shown that the inclusion of positron affects the dielectric properties of the plasma as well as the nonlinear growth rates of parametric processes. As one increases the positron density to electron density ratio from 0 to 1, maintaining quasi neutrality of the plasma, the growth rates of stimulated Raman, Brillouin, and Compton scattering processes in an isothermal plasma tend to zero due to the ponderomotive forces acting on electrons and positrons due the pump and scattered waves being equal.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Frank-van der Merwe growth in bilayer graphene

Bilayer graphene has attracted significant interest because of its unique properties, including fascinating electrical behavior when one layer is slightly rotated relative to the other. However, the quality of large-area bilayer graphene is often limited by the layer-plus-island growth mode in which islands of thicker graphene present as unavoidable impurities. Here, we report the observation of the layer-by-layer, Frank-van der Merwe (FM) growth mode in bilayer graphene where multilayer impurities are suppressed. Instead of the conventional surface adhesive energy, we found it possible to tune interface adhesive energy with an oxidative pretreatment. Finally, the FM-grown bilayer graphene is of AB stacking or with small twisting angle (θ = 0°–5°), which is more mechanically robust compared with monolayer graphene, facilitating a free-standing wet transfer technology.

36 MATERIALS SCIENCE↗

Damage buildup in multilayer hexagonal boron nitride films under Ar ion bombardment

Ion irradiation can be used to modify properties of two-dimensional hexagonal boron nitride (2D-hBN). However, the behavior of multilayer 2D-hBN under ion bombardment remains essentially unexplored. Here, in this study, we systematically study the damage buildup in 40-nm-thick multilayer 2D-hBN films irradiated at room temperature with 500 keV Ar ions with doses up to 0.64 displacements per atom. Transmission electron microscopy, soft X-ray absorption spectroscopy, and Raman spectroscopy are employed to study effects of ion irradiation. Results reveal a monotonic buildup of damage that can be described by the phenomenological zero cascade overlap model. Compared to the behavior of other group-III nitride semiconductors, radiation damage in hBN is influenced by polymorphism, involving transitions between bonding configurations of hexagonal, cubic, and amorphous phases.

Seo, M. [Lawrence Livermore National Laboratory (L↗

Cleaning graphene with a titanium sacrificial layer

Graphene is a promising material for future electronic applications and chemical vapor deposition of graphene on copper is a promising method for synthesizing graphene on the wafer scale. The processing of such graphene films into electronic devices introduces a variety of contaminants which can be difficult to remove. An approach to cleaning residues from the graphene channel is presented in which a thin layer of titanium is deposited via thermal e-beam evaporation and immediately removed. This procedure does not damage the graphene as evidenced by Raman spectroscopy, greatly enhances the electrical performance of the fabricated graphene field effect transistors, and completely removes the chemical residues from the surface of the graphene channel as evidenced by x-ray photoelectron spectroscopy.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Enhanced monolayer MoS{sub 2}/InP heterostructure solar cells by graphene quantum dots

We demonstrate significantly improved photovoltaic response of monolayer molybdenum disulfide (MoS{sub 2})/indium phosphide (InP) van der Waals heterostructure induced by graphene quantum dots (GQDs). Raman and photoluminescence measurements indicate that effective charge transfer takes place between GQDs and MoS{sub 2}, which results in n-type doping of MoS{sub 2}. The doping effect increases the barrier height at the MoS{sub 2}/InP heterojunction, thus the averaged power conversion efficiency of MoS{sub 2}/InP solar cells is improved from 2.1% to 4.1%. The light induced doping by GQD provides a feasible way for developing more efficient MoS{sub 2} based heterostructure solar cells.

14 SOLAR ENERGY↗

Studies on the structure and the magnetic properties of high-entropy spinel oxide (MgMnFeCoNi)Al 2 O 4

The study of high-entropy materials has attracted enormous interest since they could show new functional properties that are not observed in their related parent phases. Here, we report single crystal growth, structure, thermal transport, and magnetic property studies on a novel high-entropy oxide with the spinel structure (MgMnFeCoNi)Al 2 O 4 . We have successfully grown high-quality single crystals of this high-entropy oxide using the optical floating zone growth technique for the first time. The sample was confirmed to be a phase pure high-entropy oxide using x-ray diffraction and energy-dispersive spectroscopy. Through magnetization measurements, we found (MgMnFeCoNi)Al 2 O 4 exhibits a cluster spin glass state, though the parent phases show either antiferromagnetic ordering or spin glass states. Furthermore, we also found that (MgMnFeCoNi)Al 2 O 4 has much greater thermal expansion than its CoAl 2 O 4 parent compound using high resolution neutron Larmor diffraction. We further investigated the structure of this high-entropy material via Raman spectroscopy and extended x-ray absorption fine structure spectroscopy (EXAFS) measurements. From Raman spectroscopy measurements, we observed (MgMnFeCoNi)Al 2 O 4 to display a combination of the active Raman modes in its parent compounds with the modes shifted and significantly broadened. This result, together with the varying bond lengths probed by EXAFS, reveals severe local lattice distortions in this high-entropy phase. Additionally, we found a substantial decrease in thermal conductivity and suppression of the low temperature thermal conductivity peak in (MgMnFeCoNi)Al 2 O 4 , consistent with the increased lattice defects and strain. These findings advance the understanding of the dependence of thermal expansion and transport on the lattice distortions in high-entropy materials.

36 MATERIALS SCIENCE↗

Photocarrier dynamics at the interface between WS 2 and ozone-irradiated graphene

We investigate the photocarrier properties of heterostructures (HSs) formed by WS 2 and ozone-irradiated graphene (OI-graphene), with a focus on the impact of ozone irradiation. Photoluminescence and Raman spectroscopy reveal a pronounced doping effect induced by ozone irradiation on the graphene layer. Transient absorption measurements demonstrate a substantial suppression of charge transfer efficiency across the interface in the presence of ozone molecules. Spatially resolved pump-probe measurements further show a significant reduction in the diffusion coefficient of photocarriers in WS 2 on OI-graphene compared to that of individual WS 2 monolayers. The slower diffusion suggests enhanced spatial separation of electrons and holes in the WS 2 layer, induced by a built-in electric field at the interface. This effect arises from the combined influences of doping and dielectric property changes caused by ozone molecules. These findings highlight the critical influence of ozone irradiation on graphene and HS interfaces, offering valuable insights for the design of future graphene-based two-dimensional HSs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Quantum dynamics and quantum state transfer between separated nitrogen-vacancy centers embedded in photonic crystal cavities

We investigate dynamics of a laser-driven and dissipative system consisting of two nitrogen-vacancy (N-V) centers embedded in two spatially separated single-mode nanocavities in a planar photonic crystal (PC). Spontaneous emission from the excited states of the N-V centers can be effectively suppressed by virtue of the Raman transition in the dispersive regime. The system displays a series of damped oscillations under various experimental situations, where we solve the time-dependent Schroedinger equation analytically for arbitrary values of the hopping and PC-N-V coupling strengths. In particular, our results indicate that some special values should be taken for the hopping strength if we hope to have high-fidelity quantum state transfer between the two distant N-V centers. We have also analyzed the relevant entanglement dynamics in the presence of decoherence. The experimental feasibility and challenge are justified using currently available technology.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Raman-laser spectroscopy of Wannier-Stark states

Raman lasers are used as a spectroscopic probe of the state of atoms confined in a shallow one-dimensional (1D) vertical lattice. For sufficiently long laser pulses, resolved transitions in the bottom band of the lattice between Wannier Stark states corresponding to neighboring wells are observed. Couplings between such states are measured as a function of the lattice laser intensity and compared to theoretical predictions, from which the lattice depth can be extracted. Limits to the linewidth of these transitions are investigated. Transitions to higher bands can also be induced, as well as between transverse states for tilted Raman beams. All these features allow for a precise characterization of the trapping potential and for an efficient control of the atomic external degrees of freedom.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Accurate equation of state of H 2 – He binary mixtures up to 5.4 GPa

Brillouin scattering spectroscopy has been used to obtain an accurate (<1%) ρ-P equation of state (EOS) of 1:1 and 9:1 H 2 -He molar mixtures from 0.5 to 5.4 GPa at 296 K. Our calculated equations of state indicate close agreement with the experimental data right to the freezing pressure of hydrogen at 5.4 GPa. The measured velocities agree on average, within 0.5%, of an ideal mixing model. The ρ-P EOSs presented have a standard deviation of under 0.3% from the measured densities and under 1% deviation from ideal mixing. Furthermore, a detailed discussion of the accuracy, precision, and sources of error in the measurement and analyses of our equations of state is presented.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis of Yttrium Superhydride Superconductor with a Transition Temperature up to 262 K by Catalytic Hydrogenation at High Pressures

The recent observation of room-temperature superconductivity will undoubtedly lead to a surge in the discovery of new, dense, hydrogen-rich materials. The rare earth metal superhydrides are predicted to have very high-T c superconductivity that is tunable with changes in stoichiometry or doping. Here we report the synthesis of an yttrium superhydride that exhibits superconductivity at a critical temperature of 262 K at 182±8 GPa. A palladium thin film assists the synthesis by protecting the sputtered yttrium from oxidation and promoting subsequent hydrogenation. Phonon-mediated superconductivity is established by the observation of zero resistance, an isotope effect and the reduction of T c under an external magnetic field. Furthermore, the upper critical magnetic field is 103 T at zero temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗