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At least 1,081 records · Page 60

Recent applications of hard x-ray photoelectron spectroscopy

Recent applications of hard x-ray photoelectron spectroscopy (HAXPES) demonstrate its many capabilities in addition to several of its limitations. Examples are given, including measurement of buried interfaces and materials under in situ or in operando conditions, as well as measurements under x-ray standing-wave and resonant excitation. Physical considerations that differentiate HAXPES from photoemission measurements utilizing soft x-ray and ultraviolet photon sources are also presented.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetic field, frequency and temperature dependence of complex conductance of ultrathin La1.65Sr0.45CuO4/La2CuO4 films and the organic superconductors κ-(BEDT-TTF)2Cu[N(CN)2]Br

We used atomic-layer molecular beam epitaxy (ALL-MBE) to synthesize bilayer films of a cuprate metal (La1.65Sr0.45CuO4La1.65Sr0.45CuO4, LSCO) and a cuprate insulator (La2CuO4La2CuO4, LCO), in which interface superconductivity occurs in a layer that is just one-half unit cell thick. We have studied the magnetic field and temperature dependence of the complex sheet conductance, σ(ω)σ(ω), of these films, and compared them to κκ-(BEDT-TTF)2Cu[N(CN)2]Br2Cu[N(CN)2]Br single crystals. The magnetic field HH was applied both parallel and perpendicular to the 2D conducting layers. Experiments have been carried out at frequencies between 23 kHz and 50 MHz using either two-coil mutual inductance technique, or the LC resonators with spiral or rectangular coils. The real and the imaginary parts of the mutual-inductance M(T,ω)M(T,ω) between the coil and the sample were measured and converted to complex conductivity. For HH perpendicular to the conducting layers, we observed almost identical behavior in both films and κκ-Br single crystals: (i) the transition onset in the inductive response, L-1kLk-1(T) occurs at a temperature lower by 2 K than in Reσ(T)Reσ(T), (ii) this shift is almost constant with magnetic field up to 8 T; (iii) the vortex diffusion constant D(T)D(T) is exponential due to pinning of vortex cores. These results can be described by the extended dynamic theory of the Berezinski–Kosterlitz–Thouless (BKT) transition and dynamics of bound vortex–antivortex pairs with short separation lengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Neutron Scattering Studies of Classical and Quantum Fluids in Porous Media

This is an annual and the final report on DE-FG02-03ER46038 (ER46680) following a no cost extension of DE-FG02-03ER46038 from February 16, 2016 to November 15, 2016. The report period is February 16, 2016 to November 15, 2016. The contract DE-FG02-03ER46038 (ER46680) was closed on November 15, 2016. The contract institution is the University of Delaware, address: Room 210, Hullihen %%@ Hall, University of Delaware, Newark, DE 19716. The Principal Investigator is Henry R. Glyde, Department of Physics and Astronomy, University of Delaware, Newark, DE 19716 (email: glyde@udel.edu). The Administrative Point of Contact is Dale S. Weiss Tel: 302 831 3634 dsweiss@udel.edu. The DOE Program is the Office of Basic Energy %%@ Sciences, U.S. Department of Energy, Germantown Building, 1000 Independence Ave., SW Washington, DC 20585. The program manager is Dr. P. Thiyagarajan, Neutron Scattering SC-22.2/ Germantown Bldg., Tel: 301-903-9706, email: P. Thiyagarajan@Science.DOE.GOV.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Collective Energy Transport of Excitons in Two-dimensional Materials

Electronic thermal transport and thermoelectric measurements are pursued in this project to obtain unique insights into the unusual collective energy transport behaviors in two-dimensional (2D) heterostructures. Electronic thermal transport and thermoelectric measurements are essential techniques for characterizing bulk superconductors by probing the heat-carrying quasi-particles. Thermoelectric and electronic thermal transport measurements are expanded in this work beyond bulk systems to probe interactions among electrons, holes, and phonons in 2D heterostructures. In one experiment, a microbridge platform is advanced to demonstrate field-effect resistive-thermometry measurements of the electronic thermal conductivity of graphene heterostructures. Together with first principles theoretical calculations and analytical models, the experimental results suggest that tunable electron coupling with flexural phonons provides a knob to control quantum matters in graphene heterostructures with broken reflection symmetry. In another experiment, the Seebeck coefficient (S) is measured to probe interlayer interactions in electron-hole bilayers that are predicted to give rise to the emergence of a variety of correlated states. As a measure of the entropy, the measured S reveals the signature of electric injection of interlayer excitons in transition metal dichalcogenide (TMD) structures.

36 MATERIALS SCIENCE↗

Four-dimensional electrical conductivity monitoring of stage-driven river water intrusion: Accounting for water table effects using a transient mesh boundary and conditional inversion constraints

Our paper describes and demonstrates two methods of providing a priori information to the surface-based time-lapse three-dimensional electrical resistivity tomography (ERT) problem for monitoring stage-driven or tide-driven surface water intrusion into aquifers. First, a mesh boundary is implemented that conforms to the known location of the water table through time, thereby enabling the inversion to place a sharp bulk conductivity contrast at that boundary without penalty. Moreover, a nonlinear inequality constraint is used to allow only positive or negative transient changes in EC to occur within the saturated zone, dependent on the relative contrast in fluid electrical conductivity between surface water and groundwater. A 3-D field experiment demonstrates that time-lapse imaging results using traditional smoothness constraints are unable to delineate river water intrusion. The water table and inequality constraints provide the inversion with the additional information necessary to resolve the spatial extent of river water intrusion through time.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electrical properties of methane hydrate + sediment mixtures: The σ of CH 4 Hydrate + Sediment

Knowledge of the electrical properties of multicomponent systems with gas hydrate, sediments, and pore water is needed to help relate electromagnetic (EM) measurements to specific gas hydrate concentration and distribution patterns in nature. We built a pressure cell capable of measuring in situ electrical properties of multicomponent systems such that the effects of individual components and mixing relations can be assessed. We first established the temperature-dependent electrical conductivity (σ) of pure, single-phase methane hydrate to be ~5 orders of magnitude lower than seawater, a substantial contrast that can help differentiate hydrate deposits from significantly more conductive water-saturated sediments in EM field surveys. We report σ measurements of two-component systems in which methane hydrate is mixed with variable amounts of quartz sand or glass beads. Sand by itself has low σ but is found to increase the overall σ of mixtures with well-connected methane hydrate. Alternatively, the overall σ decreases when sand concentrations are high enough to cause gas hydrate to be poorly connected, indicating that hydrate grains provide the primary conduction path. Our measurements suggest that impurities from sand induce chemical interactions and/or doping effects that result in higher electrical conductivity with lower temperature dependence. Finally, these results can be used in the modeling of massive or two-phase gas-hydrate-bearing systems devoid of conductive pore water. Further experiments that include a free water phase are the necessary next steps toward developing complex models relevant to most natural systems.

03 NATURAL GAS↗

Interactions among hydraulic conductivity distributions, subsurface topography, and transport thresholds revealed by a multitracer hillslope irrigation experiment

Interactions among hydraulic conductivity distributions, subsurface topography, and lateral flow are poorly understood. We applied 407 mm of water and a suite of tracers over 51 h to a 12 by 16.5 m forested hillslope segment to determine interflow thresholds, preferential pathway pore velocities, large-scale conductivities, the time series of event water fractions, and the fate of dissolved nutrients. The 12% hillslope featured loamy sand A and E horizons overlying a sandy clay loam Bt at 1.25 m average depth. Interflow measured from two drains within an interception trench commenced after 131 and 208 mm of irrigation. Cumulative interflow equaled 49% of applied water. Conservative tracer differences between the collection drains indicated differences in flow paths and storages within the plot. Event water fractions rose steadily throughout irrigation, peaking at 50% sixteen h after irrigation ceased. Data implied that tightly held water exchanged with event water throughout the experiment and a substantial portion of preevent water was released from the argillic layer. Surface-applied dye tracers bypassed the matrix, with peak concentrations measured shortly after flow commencement, indicating preferential network conductivities of 864–2240 mm/h, yet no macropore flow was observed. Near steady-state flow conditions indicated average conductivities of 460 mm/h and 2.5 mm/h for topsoils and the Bt horizon, respectively. Low ammonium and phosphorus concentrations in the interflow suggested rapid uptake or sorption, while higher nitrate concentrations suggested more conservative transport. Lastly, these results reveal how hydraulic conductivity variation and subsurface topographic complexity explain otherwise paradoxical solute and flow behaviors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Direct evidence for EMIC wave scattering of relativistic electrons in space: EMIC-Driven Electron Losses in Space

Electromagnetic ion cyclotron (EMIC) waves have been proposed to cause efficient losses of highly relativistic (>1 MeV) electrons via gyroresonant interactions. Simultaneous observations of EMIC waves and equatorial electron pitch angle distributions, which can be used to directly quantify the EMIC wave scattering effect, are still very limited, however. In the present study, we evaluate the effect of EMIC waves on pitch angle scattering of ultrarelativistic (>1 MeV) electrons during the main phase of a geomagnetic storm, when intense EMIC wave activity was observed in situ (in the plasma plume region with high plasma density) on both Van Allen Probes. EMIC waves captured by Time History of Events and Macroscale Interactions during Substorms (THEMIS) probes and on the ground across the Canadian Array for Real-time Investigations of Magnetic Activity (CARISMA) are also used to infer their magnetic local time (MLT) coverage. From the observed EMIC wave spectra and local plasma parameters, we compute wave diffusion rates and model the evolution of electron pitch angle distributions. In conclusion, by comparing model results with local observations of pitch angle distributions, we show direct, quantitative evidence of EMIC wave-driven relativistic electron losses in the Earth’s outer radiation belt.

58 GEOSCIENCES↗

Record-Breaking Magnetoresistance at the Edge of a Microflake of Natural Graphite

Placing several electrodes at the edge of a micrometer-size Sri Lankan natural graphite sample at distances comparable to the size of the internal crystalline regions, we found record values for the change of the resistance with magnetic field. At low temperatures and at B ~ 21 T the magnetoresistance (MR) reaches ≈ 10 7 %. The MR values exceed by far all earlier reported ones for graphite and they are comparable or even larger (at T > 50 K) than the largest reported in solids including the Weyl semimetals. The origin of this large MR lies in the existence of highly conducting 2D interfaces aligned parallel to the graphene planes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strain tuning and strong enhancement of ionic conductivity in SrZrO 3 -RE 2 O 3 (RE = Sm, Eu, Gd, Dy, and Er) nanocomposite films

Fast ion transport channels at interfaces in thin films have attracted great attention due to a range of potential applications for energy materials and devices, for, solid oxide fuel cells, sensors, and memories. Here, it is shown that in vertical nanocomposite heteroepitaxial films of SrZrO 3 –RE 2 O 3 (RE = Sm, Eu, Gd, Dy, and Er) the ionic conductivity of the composite can be tuned and strongly enhanced using embedded, stiff, and vertical nanopillars of RE 2 O 3 . With increasing lattice constant of RE 2 O 3 from Er 2 O 3 to Sm 2 O 3 , it is found that the tensile strain in the SrZrO 3 increases proportionately, and the ionic conductivity of the composite increases accordingly, by an order of magnitude. Lastly, the results here conclusively show, for the first time, that strain in films can be effectively used to tune the ionic conductivity of the materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Penta-Twinned Copper Nanorods: Facile Synthesis via Seed-Mediated Growth and Their Tunable Plasmonic Properties

When seed-mediated growth is used as a versatile approach to the synthesis of penta-twinned Cu nanorods with uniform diameters and controllable aspect ratios is reported. The success of this approach relies on our recent synthesis of uniform Pd decahedra, with sizes in the range of 6–20 nm. The Pd decahedral seeds can direct the heterogeneous nucleation and growth of Cu along the fivefold axis to produce nanorods with uniform diameters defined by the lateral dimension of the original seeds. Due to a large mismatch in the lattice constants between Cu and Pd (7.1%), the deposited Cu is forced to grow along one side of the Pd decahedral seed, generating a nanorod with an asymmetric distribution of Cu, with the Pd seed situated at one of the two ends. According to extinction spectra, the as-obtained Cu nanorods can be stored in water under the ambient conditions for at least six months without noticeable degradation. The resulting stability allows us to systematically investigate the size-dependent surface plasmon resonance properties of the penta-twinned Cu nanorods. With the nanorod transverse modes positioned at 560 nm, the longitudinal modes can be readily tuned from the visible to the near-infrared region by controlling the aspect ratio.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ionic Liquid Activation of Amorphous Metal-Oxide Semiconductors for Flexible Transparent Electronic Devices

To begin this abstract, amorphous metal-oxide semiconductors offer the high carrier mobilities and excellent large-area uniformity required for high performance, transparent, flexible electronic devices; however, a critical bottleneck to their widespread implementation is the need to activate these materials at high temperatures which are not compatible with flexible polymer substrates. The highly controllable activation of amorphous indium gallium zinc oxide semiconductor channels using ionic liquid gating at room temperature is reported. Activation is controlled by electric field-induced oxygen migration across the ionic liquid-semiconductor interface. In addition to activation of unannealed devices, it is shown that threshold voltages of a transistor can be linearly tuned between the enhancement and depletion modes. Finally, the first ever example of transparent flexible thin film metal oxide transistor on a polyamide substrate created using this simple technique is demonstrated. Finally, this study demonstrates the potential of field-induced activation as a promising alternative to traditional postdeposition thermal annealing which opens the door to wide scale implementation into flexible electronic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis and characterization of 2D molybdenum carbide (MXene)

Large scale synthesis and delamination of 2D Mo 2 CT x (where T is a surface termination group) has been achieved by selectively etching gallium from the recently discovered nanolaminated, ternary transition metal carbide Mo 2 Ga 2 C. Different synthesis and delamination routes result in different flake morphologies. The resistivity of free-standing Mo 2 CT x films increases by an order of magnitude as the temperature is reduced from 300 to 10 K, suggesting semiconductor-like behavior of this MXene, in contrast to Ti 3 C 2 T x which exhibits metallic behavior. At 10 K, the magnetoresistance is positive. Additionally, changes in electronic transport are observed upon annealing of the films. When 2 μm thick films are tested as electrodes in supercapacitors, capacitances as high as 700 F cm –3 in a 1 m sulfuric acid electrolyte and high capacity retention for at least 10,000 cycles at 10 A g –1 are obtained. Free-standing Mo 2 CT x films, with ≈8 wt% carbon nanotubes, perform well when tested as an electrode material for Li-ions, especially at high rates. In conclusion, at 20 and 131 C cycling rates, stable reversible capacities of 250 and 76 mAh g –1 , respectively, are achieved for over 1000 cycles.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ferroelectric Self-Poling, Switching, and Monoclinic Domain Configuration in BiFeO 3 Thin Films

Self-poling of ferroelectric films, i.e., a preferred, uniform direction of the ferroelectric polarization in as-grown samples is often observed yet poorly understood despite its importance for device applications. The multiferroic perovskite BiFeO 3 , which crystallizes in two distinct structural polymorphs depending on applied epitaxial strain, is well known to exhibit self-poling. This study investigates the effect of self-poling on the monoclinic domain configuration and the switching properties of the two polymorphs of BiFeO 3 (R' and T') in thin films grown on LaAlO 3 substrates with slightly different La 0.3 Sr 0.7 MnO 3 buffer layers. Our study shows that the polarization state formed during the growth acts as “imprint” on the polarization and that switching the polarization away from this self-poled direction can only be done at the expense of the sample's monoclinic domain configuration. We observed reduction of the monoclinic domain size and found that it was largely reversible; hence, the domain size is restored when the polarization is switched back to its original orientation. This is a direct consequence of the growth taking place in the polar phase (below T c ). Finally, switching the polarization away from the preferred configuration, in which defects and domain patterns synergistically minimize the system's energy, leads to a domain state with smaller (and more highly strained and distorted) monoclinic domains.

36 MATERIALS SCIENCE↗

Enhanced Thermoelectric Performance in 18-Electron Nb 0.8 CoSb Half-Heusler Compound with Intrinsic Nb Vacancies

Typical 18-electron half-Heusler compounds, ZrNiSn and NbFeSb, are identified as promising high-temperature thermoelectric materials. NbCoSb with nominal 19 valence electrons, which is supposed to be metallic, is recently reported to also exhibit thermoelectric properties of a heavily doped n-type semiconductor. Here for the first time, it is experimentally demonstrated that the nominal 19-electron NbCoSb is actually the composite of 18-electron Nb 0.8 +δCoSb (0 ≤ δ < 0.05) and impurity phases. Single-phase Nb 0.8δ +CoSb with intrinsic Nb vacancies, following the 18-electron rule, possesses improved thermoelectric performance, and the slight change in the content of Nb vacancies has a profound effect on the thermoelectric properties. The carrier concentration can be controlled by varying the Nb deficiency, and the optimization of the thermoelectric properties can be realized within the narrow pure phase region. Benefiting from the elimination of impurity phases and the optimization of carrier concentration, thermoelectric performance is remarkably enhanced by ≈100% and a maximum zT of 0.9 is achieved in Nb 0.83 CoSb at 1123 K. Here, this work expands the family of half-Heusler thermoelectric materials and opens a new avenue for searching for nominal 19-electron half-Heusler compounds with intrinsic vacancies as promising thermoelectric materials.

36 MATERIALS SCIENCE↗

All-Solid-State Synaptic Transistor with Ultralow Conductance for Neuromorphic Computing

Electronic synaptic devices are important building blocks for neuromorphic computational systems that can go beyond the constraints of von Neumann architecture. Although two-terminal memristive devices are demonstrated to be possible candidates, they suffer from several shortcomings related to the filament formation mechanism including nonlinear switching, write noise, and high device conductance, all of which limit the accuracy and energy efficiency. Electrochemical three-terminal transistors, in which the channel conductance can be tuned without filament formation provide an alternative platform for synaptic electronics. In this work, an all-solid-state electrochemical transistor made with Li ion–based solid dielectric and 2D α-phase molybdenum oxide (α-MoO 3 ) nanosheets as the channel is demonstrated. These devices achieve nonvolatile conductance modulation in an ultralow conductance regime (<75 nS) by reversible intercalation of Li ions into the α-MoO 3 lattice. Based on this operating mechanism, the essential functionalities of synapses, such as short- and long-term synaptic plasticity and bidirectional near-linear analog weight update are demonstrated. Simulations using the handwritten digit data sets demonstrate high recognition accuracy (94.1%) of the synaptic transistor arrays. These results provide an insight into the application of 2D oxides for large-scale, energy-efficient neuromorphic computing networks.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Atom–by–Atom Fabrication of Single and Few Dopant Quantum Devices

Atomically precise fabrication has an important role to play in developing atom-based electronic devices for use in quantum information processing, quantum materials research, and quantum sensing. Atom-by-atom fabrication has the potential to enable precise control over tunnel coupling, exchange coupling, on-site charging energies, and other key properties of basic devices needed for solid-state quantum computing and analog quantum simulation. Using hydrogen-based scanning probe lithography, individual dopant atoms are deterministically placed relative to atomically aligned contacts and gates to build single electron transistors, single atom transistors, and gate-controlled quantum sensing devices. Here, the key steps required to fabricate and demonstrate the essential building blocks needed for spin selective initialization/readout and coherent quantum manipulation are described.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Controlled Nucleation and Stabilization of Ferroelectric Domain Wall Patterns in Epitaxial (110) Bismuth Ferrite Heterostructures

Ferroelectric domain walls, topological entities separating domains of uniform polarization, are promising candidates as active elements for nanoscale memories. In such applications, controlled nucleation and stabilization of domain walls are critical. In this work, using in situ transmission electron microscopy and phase-field simulations, a controlled nucleation of vertically oriented 109° domain walls in (110)-oriented BiFeO 3 (BFO) thin films is reported. In the switching experiment, reversed domains that are nucleated preferentially at the nanoscale edges of the “crest and sag” pattern-like electrode under external bias subsequently grow into a stable stripe configuration. In addition, when triangular pockets (with an in-plane polarization component) are present, these domain walls are pinned to form stable flux-closure domains. Phase field simulations show that i) field enhancement at the edges of the electrode causes site-specific domain nucleation, and ii) the local electrostatics at the domain walls drives the formation of flux closure domains, thus stabilizing the striped pattern, irrespective of the initial configuration. The results demonstrate how flux closure pinning can be exploited in conjunction with electrode patterning and substrate orientation to achieve a desired topological defect configuration. These insights constitute critical advancements in exploiting domain walls in next generation ferroelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗