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At least 109 records · Page 6

Many-Body Exciton and Intervalley Correlations in Heavily Electron-Doped WSe 2 Monolayers

We shoe that in monolayer transition-metal dichalcogenide semiconductors, many-body correlations can manifest in optical spectra when electron-hole pairs (excitons) are photoexcited into a 2D Fermi sea of mobile carriers. At low carrier densities, the formation of charged excitons (X ± ) is well documented. However, in WSe 2 monolayers, an additional absorption resonance, often called X -' , emerges at high electron density. Its origin is not understood. Here, we investigate the X -' state via polarized absorption spectroscopy of gated WSe 2 monolayers in magnetic fields to 60T. Field-induced filling and emptying of the lowest optically active Landau level in the K ' valley causes repeated quenching of the corresponding optical absorption. Surprisingly, these quenchings are accompanied by absorption changes to higher Landau levels in both K ' and K valleys, which are unoccupied. These results cannot be reconciled within a single-particle picture, and demonstrate the many-body nature and intervalley correlations of the X -' quasiparticle state.

2D materials↗

Lithiation Induced Phases in 1T'-MoTe 2 Nanoflakes

Multiple polytypes of MoTe 2 with distinct structures and intriguing electronic properties can be accessed by various physical and chemical approaches. Here, in this study, we report electrochemical lithium (Li) intercalation into 1T'-MoTe 2 nanoflakes, leading to the discovery of two previously unreported lithiated phases. Distinguished by their structural differences from the pristine 1T' phase, these distinct phases were characterized using in situ polarization Raman spectroscopy and in situ single-crystal X-ray diffraction. The lithiated phases exhibit increasing resistivity with decreasing temperature, and their carrier densities are two to 4 orders of magnitude smaller than the metallic 1T' phase, as probed through in situ Hall measurements. The discovery of these gapped phases in initially metallic 1T'-MoTe 2 underscores electrochemical intercalation as a potent tool for tuning the phase stability and electron density in two-dimensional (2D) materials.

36 MATERIALS SCIENCE↗

Observing the Surface Termination of LaScO 3 Perovskite Using Solid-State Nuclear Magnetic Resonance

Materials with well-defined surfaces are drawing increased attention for the design of bespoke catalysts and nanomaterials. Gaining a detailed understanding of the surfaces of these materials is an important challenge, which is often complicated by surface polymorphism and dynamic restructuring. We introduce the use of surface-enhanced NMR spectroscopy for the observation of such surfaces, focusing on LaScO 3 as an example. Here, we show that double-resonance NMR experiments correlating surface oxygen and probe molecules to the 139 La and 45 Sc nuclei at the surface reveal the material to be terminated by a ScO x monolayer. Surface-selective 17 O and 45 Sc NMR experiments further showed the material to be hydroxyl terminated and that the surface may be prone to dynamic restructuring as a result of moisture exposure. Perhaps most interestingly, surface-selective 139 La NMR experiments revealed the existence of previously undetected surface lanthanum defects, suggesting that surface-enhanced NMR may be useful as a guide in the synthesis of defect-free surfaces in the design of various nanomaterials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Novel design for a polarizing DUV spectrometer using a Wollaston prism and its application as a diagnostic for measuring Thomson scattering data in the presence of strong self-emission backgrounds

We present a novel design for an optical spectrometer for use in ultraviolet Thomson scattering measurements of plasma parameters in high energy density (HED) inertial confinement fusion experiments on large-scale high-energy laser facilities. In experiments investigating high-Z plasmas, the fidelity of measurements is commonly limited by signal/background ratios approaching or exceeding unity. An alpha barium borate Wollaston prism can provide both spectral dispersion and polarization channel separation, allowing simultaneous measurement of both the Thomson scattering signal and plasma self-emission along a single line of sight and in a single experiment, which should greatly improve data quality and reduce the opportunity cost of taking high quality measurements. Here, we present a basic discussion of the design and a worked example of an instrument designed to take fourth harmonic electron plasma wave measurements in HED experiments at the OMEGA laser facility.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Comparing Theoretical Salt Concentration Profiles in a Polymer Electrolyte with Experimental Measurements using Operando Raman Spectroscopy

Concentrated solution theory has furthered our understanding of ion transport in electrolytes. This theory can be used to predict salt concentration profiles under an applied current if the transport properties of the electrolyte (conductivity ( κ ), restricted diffusion coefficient ( D ), and the cation transference number with respect to the solvent velocity ( t + 0 )), and the thermodynamic factor ( T f ) are known. In this work, we provide the first study comparing the predicted salt concentration profiles with measurements based on operando Raman spectroscopy. Concentration polarization is asymmetrical; the increase in salt concentration near the positive electrode is a factor of two greater than the decrease in salt concentration near the negative electrode. We find qualitative agreement between theory and experiment. Further work is needed to resolve the quantitative differences.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exploring the Effectiveness of Carbon Cloth Electrodes for All-Vanadium Redox Flow Batteries

Vanadium redox flow batteries (VRFBs) have shown to be a promising technology for integrating intermittent renewable energy sources into the existing electrical grid. Incorporation of carbon cloth electrodes into VRFB is an area of interest for their enhanced electrochemical performance, however, issues with performance degradation throughout the duration of the experiment persist. This study investigates the performance evolution of carbon cloth electrodes during VRFB cycling to build a hypothesis on possible reasons for the declining performance. Electrochemical impedance spectroscopy and polarization curve measurements are used in conjunction to monitor the electrode degradation and shed light on the effectiveness of carbon cloth electrodes during extended cycling experiments. A detailed investigation into the structure of the carbon cloth electrodes before and after cycling, via several material characterization tests, provides insight needed to determine an explanation for the increasing resistance. The structural integrity and surface morphology of the carbon cloth electrodes are evaluated to compare the electrode before and after cycling, displaying any changes to the electrode due to cycling. Durability of hydrophilicity during RFB cycling is found to be a key feature for future carbon cloth electrode design efforts.

25 ENERGY STORAGE↗

Single-Crystal X-ray Spectropolarimeter

This presentation will be presented during the MSTS Science and Technology Work in Progress Seminar Webex meeting scheduled for Tuesday, November 17, 2020.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Tunable lasers and their application in analytical chemistry

The impact that laser techniques might have in chemical analysis is examined. Absorption, scattering, and heterodyne detection is considered. Particular emphasis is placed on the advantages of using frequency-tunable sources, and dye solution lasers are regarded as the outstanding example of this type of laser. Types of spectroscopy that can be carried out with lasers are discussed along with the ultimate sensitivity or minimum detectable concentration of molecules that can be achieved with each method. Analytical applications include laser microprobe analysis, remote sensing and instrumental methods such as laser-Raman spectroscopy, atomic absorption/fluorescence spectrometry, fluorescence assay techniques, optoacoustic spectroscopy, and polarization measurements. The application of lasers to spectroscopic methods of analysis would seem to be a rewarding field both for research in analytical chemistry and for investments in instrument manufacturing.

Steinfeld, J. I.↗

Photometry and spectroscopy of a newly discovered polar - Nova Cygni 1975 (V1500 CYG)

The paper reports photometric and spectroscopic observations which led to the conclusion that Nova Cygni 1975 (V1500 Cyg) is a polar (of AM Her-type).The CCD photometry confirms the constancy of the photometric period which is again interpreted as an orbital cycle. The time-resolved MMT spectra make it possible to reconstruct, under several assumptions, the basic system parameters: M1=0.9M solar mass and M2=0.31M solar mass.

Kaluzny, Janusz↗

Mars: Compositional variability of ferric/ferrous minerals and polar volatiles from groundbased imaging spectroscopy

In an attempt to further constrain the ferric and ferrous mineralogy of Mars, Bell et al. (1989; 1990) obtained high resolution imaging spectroscopic data of much of the Martian surface in the visible and near-infrared (0.4-1.1 micron) during the 1988 opposition. Preliminary analysis of these data showed further evidence of crystalline hematite absorption features at 0.8-0.9 microns and 0.6-0.7 microns. Additionally, the 0.6-0.7 micron Fe(III) band was shown to vary across the surface, with a substantial correlation with albedo in the region studied. Calibration of this 1988 data set (along with a similar data set obtained during the 1990 opposition) has been ongoing, and some of the most recent results of the analysis of these data using linear spectral mixture modeling are reported.

Bell, James F., III↗

Aligned Single Wall Carbon Nanotube Polymer Composites Using an Electric Field

While high shear alignment has been shown to improve the mechanical properties of single wall carbon nanotubes (SWNT)-polymer composites, it is difficult to control and often results in degradation of the electrical and dielectric properties of the composite. Here, we report a novel method to actively align SWNTs in a polymer matrix, which allows for control over the degree of alignment of SWNTs without the side effects of shear alignment. In this process, SWNTs are aligned via field-induced dipolar interactions among the nanotubes under an AC electric field in a liquid matrix followed by immobilization by photopolymerization while maintaining the electric field. Alignment of SWNTs was controlled as a function of magnitude, frequency, and application time of the applied electric field. The degree of SWNT alignment was assessed using optical microscopy and polarized Raman spectroscopy and the morphology of the aligned nanocomposites was investigated by high resolution scanning electron microscopy. The structure of the field induced aligned SWNTs is intrinsically different from that of shear aligned SWNTs. In the present work, SWNTs are not only aligned along the field, but also migrate laterally to form thick, aligned SWNT percolative columns between the electrodes. The actively aligned SWNTs amplify the electrical and dielectric properties in addition to improving the mechanical properties of the composite. All of these properties of the aligned nanocomposites exhibited anisotropic characteristics, which were controllable by tuning the applied field conditions.

Park, Cheol↗

Carbonatite metasomatism and water systematics of peridotite xenoliths from Lanzarote, Canaries

Water in Earth’s mantle, present as structural hydrogen in minerals, influences large scale processes like mantle deformation, plate tectonics, and melting. To better understand the processes controlling water concentrations in the Earth’s upper mantle, we analyzed hydrogen (calculated as ppm wt. H2O), major, and trace element concentrations in minerals from harzburgite xenoliths of Lanzarote, Canaries. Previous studies have shown evidence for carbonatite metasomatism in Lanzarote peridotites and carbonatite magmas have erupted in the Canaries. Thus, the Canaries offer a rare opportunity to examine the role of metasomatism and carbonatitic magmas in rehydrating the oceanic lithosphere during plume-lithosphere interaction. Major element data (obtained by electron microprobe) show that these peridotites are highly depleted compared to the primitive mantle, with a high average olivine Mg# (91.1 ± 0.5), low bulk rock Al2O3 (0.4 to 1.4 wt.%), high spinel Cr# (40 to 72) from which high degrees of melting were estimated (15 to 21%). There is no evidence of hydrous phases (e.g., amphibole and phlogopite), thus water in these peridotites is thought to be stored only in nominally anhydrous minerals and melt inclusions. Water concentrations (determined by polarized FTIR spectroscopy), in the peridotite silicate minerals range from 2.7 to 13 ppm in olivine, 42 to 265 ppm in orthopyroxene (Opx), and 76 to 470 ppm in clinopyroxene (Cpx). Reconstructed bulk rock water concentrations range from 5 to 115 ppm, generally lower than estimates for the depleted mantle (DM, 50-200 ppm). Trace element data in Opx, Cpx, and bulk rock frequently show high La/Yb ratios (up to 12.2, 71.5, 45.2; respectively) and strong negative Zr, Hf, and Ti anomalies relative to REE, consistent with carbonatite metasomatism. With decreasing Ti/Eucpx ratios, a proxy for carbonatite metasomatism, the bulk water increases. The calculated trace element compositions of melts in equilibrium with Cpx strongly resemble those of carbonatites. However, the bulk rock water concentrations are two magnitudes lower than what is expected by equilibrium with a carbonatite melt. Evidently, carbonatitic metasomatism did rehydrate of the Lanzarote mantle lithosphere but less so than expected, implying lower partitioning of H in the presence of CO2than a silicate melt.

S. Patterson↗

Polarization-resolved core exciton dynamics in LiF using attosecond transient absorption spectroscopy

The ability to control absorption by modifying the polarization of light presents an exciting opportunity to experimentally determine the orbital alignment of absorption features. Here, attosecond extreme ultraviolet (XUV) transient absorption spectroscopy is used to investigate the polarization dependence of core exciton dynamics in LiF thin films at the Li + K edge. XUV pulses excite electrons from the Li 1s core level into the conduction band, allowing for the formation of a p-orbital-like core exciton, aligned along the XUV light polarization axis. A sub-5 fs near-infrared (NIR) probe pulse then arrives at variable time delays, perturbing the XUV-excited states and allowing the coherence decay of the core exciton to be mapped. The coherence lifetimes are found to be ≈ 2.4 ± 0.4 fs, which is attributed to a phonon-mediated dephasing mechanism as in previous core exciton studies. The differential absorption features are also shown to be sensitive to the relative polarization of the XUV and NIR fields. The parallel NIR probe induces couplings between the initial XUV-excited p-like bright exciton and s-like dark excitons. When crossed pump and probe polarizations are used, the coupling between the bright and dark states is no longer dipole-allowed, and the transient absorption signal associated with the coupling is suppressed by approximately 90%. This interpretation is supported by simulations of a few-level model system, as well as analysis of the calculated band structure. Here, the results indicate that laser polarization can serve as a powerful experimental tool for exploring the orbital alignment of core excitonic states in solid-state materials.

Attosecond laser spectroscopy↗