RESUMEN
A three-dimensional strong-topological insulator or semimetal hosts topological surface states which are often said to be gapless so long as time-reversal symmetry is preserved. This narrative can be mistaken when surface state degeneracies occur away from time-reversal-invariant momenta. The mirror invariance of the system then becomes essential in protecting the existence of a surface Fermi surface. Here we show that such a case exists in the strong-topological-semimetal Bi(4)Se(3). Angle-resolved photoemission spectroscopy and ab initio calculations reveal partial gapping of surface bands on the Bi(2)Se(3) termination of Bi(4)Se(3)(111), where an 85 meV gap along ΓÌ KÌ closes to zero toward the mirror-invariant ΓÌ MÌ azimuth. The gap opening is attributed to an interband spin-orbit interaction that mixes states of opposite spin helicity.
RESUMEN
Proximity-induced superconductivity in a 3D topological insulator represents a new avenue for observing zero-energy Majorana fermions inside vortex cores. Relatively small gaps and low transition temperatures of conventional s-wave superconductors put hard constraints on these experiments. Significantly larger gaps and higher transition temperatures in cuprate superconductors might be an attractive alternative to considerably relax these constraints, but it is not clear whether the proximity effect would be effective in heterostructures involving cuprates and topological insulators. Here, we present angle-resolved photoemission studies of thin Bi(2)Se(3) films grown in situ on optimally doped Bi(2)Sr(2)CaCu(2)O(8+δ) substrates that show the absence of proximity-induced gaps on the surfaces of Bi(2)Se(3) films as thin as a 1.5 quintuple layer. These results suggest that the superconducting proximity effect between a cuprate superconductor and a topological insulator is strongly suppressed, likely due to a very short coherence length along the c axis, incompatible crystal and pairing symmetries at the interface, small size of the topological surface state's Fermi surface, and adverse effects of a strong spin-orbit coupling in the topological material.
RESUMEN
The electronic and chemical structure of the metal-to-semiconductor interface was studied by photoemission spectroscopy for evaporated Cr, Ti, Al and Cu overlayers on sputter-cleaned as-deposited and thermally treated thin films of amorphous hydrogenated boron carbide (a-B(x)C:H(y)) grown by plasma-enhanced chemical vapor deposition. The films were found to contain ~10% oxygen in the bulk and to have approximate bulk stoichiometries of a-B(3)CO(0.5):H(y). Measured work functions of 4.7/4.5 eV and valence band maxima to Fermi level energy gaps of 0.80/0.66 eV for the films (as-deposited/thermally treated) led to predicted Schottky barrier heights of 1.0/0.7 eV for Cr, 1.2/0.9 eV for Ti, 1.2/0.9 eV for Al, and 0.9/0.6 eV for Cu. The Cr interface was found to contain a thick partial metal oxide layer, dominated by the wide-bandgap semiconductor Cr(2)O(3), expected to lead to an increased Schottky barrier at the junction and the formation of a space-charge region in the a-B(3)CO(0.5):H (y) layer. Analysis of the Ti interface revealed a thick layer of metal oxide, comprising metallic TiO and Ti (2)O (3), expected to decrease the barrier height. A thinner, insulating Al(2)O(3) layer was observed at the Al-to-a-B(3)CO(0.5):H(y) interface, expected to lead to tunnel junction behavior. Finally, no metal oxides or other new chemical species were evident at the Cu-to-a-B(3)CO(0.5):H(y) interface in either the core level or valence band photoemission spectra, wherein characteristic metallic Cu features were observed at very thin overlayer coverages. These results highlight the importance of thin-film bulk oxygen content on the metal-to-semiconductor junction character as well as the use of Cu as a potential Ohmic contact material for amorphous hydrogenated boron carbide semiconductor devices such as high-efficiency direct-conversion solid-state neutron detectors.
RESUMEN
Magic angle spinning solid-state nuclear magnetic resonance spectroscopy techniques are applied to the elucidation of the local physical structure of an intermediate product in the plasma-enhanced chemical vapour deposition of thin-film amorphous hydrogenated boron carbide (B(x)C:H(y)) from an orthocarborane precursor. Experimental chemical shifts are compared with theoretical shift predictions from ab initio calculations of model molecular compounds to assign atomic chemical environments, while Lee-Goldburg cross-polarization and heteronuclear recoupling experiments are used to confirm atomic connectivities. A model for the B(x)C:H(y) intermediate is proposed wherein the solid is dominated by predominantly hydrogenated carborane icosahedra that are lightly cross-linked via nonhydrogenated intraicosahedral B atoms, either directly through B-B bonds or through extraicosahedral hydrocarbon chains. While there is no clear evidence for extraicosahedral B aside from boron oxides, â¼40% of the C is found to exist as extraicosahedral hydrocarbon species that are intimately bound within the icosahedral network rather than in segregated phases.
RESUMEN
Detection of neutrons, at high total efficiency, with greater resolution in kinetic energy, time and/or real-space position, is fundamental to the advance of subfields within nuclear medicine, high-energy physics, non-proliferation of special nuclear materials, astrophysics, structural biology and chemistry, magnetism and nuclear energy. Clever indirect-conversion geometries, interaction/transport calculations and modern processing methods for silicon and gallium arsenide allow for the realization of moderate- to high-efficiency neutron detectors as a result of low defect concentrations, tuned reaction product ranges, enhanced effective omnidirectional cross sections and reduced electron-hole pair recombination from more physically abrupt and electronically engineered interfaces. Conversely, semiconductors with high neutron cross sections and unique transduction mechanisms capable of achieving very high total efficiency are gaining greater recognition despite the relative immaturity of their growth, lithographic processing and electronic structure understanding. This review focuses on advances and challenges in charged-particle-based device geometries, materials and associated mechanisms for direct and indirect transduction of thermal to fast neutrons within the context of application. Calorimetry- and radioluminescence-based intermediate processes in the solid state are not included.
Asunto(s)
Neutrones , Fenómenos Físicos , Electrones , CinéticaRESUMEN
Systematic investigation of the ligand exchange reactions between manganese(II) acetate and benzoic acid under solvothermal conditions led to the isolation of crystalline complexes {Mn5(OC(O)CH3)6(OC(O)C6H5)4}(infinity) ( 1) and {Mn5(OC(O)CH3)4(OC(O)C6H5)6}}(infinity) ( 2) in high (i.e., >90%) yields. The complexes are characterized structurally as 2-D honeycomb-like sheets comprised of edge-shared Mn 12 loops with some noteworthy differences as follows. First, buckling of the 2-D sheet in 1 is not observed for 2, presumably as a consequence of additional intersheet phenyl groups in the latter. Second, complex 1 is comprised of only six-coordinate MnII, while 2 has both pseudo-octahedral and distorted trigonal bipyramidal coordinate metal ions. Third, while complex 2 exhibits pi-stacking interactions with intersheet phenyl-phenyl contacts of 3.285 and 3.369 A, 1 exhibits no such bonding. Antiferromagnetic exchange is observed with Weiss constants (theta) of -28 and -56 K and Neel temperatures of 2.2 and 8.2 K for complexes 1 and 2, respectively. The paramagnetic transition at higher temperatures for complex 2 may be attributed to pi-pi exchange through phenyl groups in adjacent layers. Preliminary gas sorption studies (76 K) indidate preferential adsorption of H2 versus N2 for complex 1 only.
RESUMEN
We compare the molecular films of three different isomers of closo-dicarbadodecaborane (orthocarborane (1,2-C2B10H12), metacarborane (1,7-C2B10H12), paracarborane (1,12-C2B10H12)) and two related icosahedral cage molecules, 1-phospha-2-carbadodecaborane (1,2-PCB10H11) and 1-phospha-7-carbadodecaborane (1,7-PCB10H11) adsorbed on a variety of substrates. While the experimental electronic structure from combined photoemission and inverse photoemission studies of the molecular films are in good agreement with semiempirical calculations for the isolated molecule, there is a shift in the chemical potential for each molecule. The experimental position of the molecular chemical potential implicates an influence of both interface and adsorbate dipole.
RESUMEN
We present, herein, an extended study of the half-Heusler alloy NiMnSb, starting with the deposition technique, continuing with the basic structural and magnetic properties of the thin films, and finishing with the electronic and compositional properties of their surfaces. The experimental methods we apply combine magnetization and magnetoresistivity measurements, atomic force microscopy, ferromagnetic resonance, x-ray and neutron diffraction, low energy electron diffraction, angle resolved x-ray photoemission, extended x-ray absorption fine structure spectroscopy, soft x-ray magnetic circular dichroism and spin polarized inverse photoemission spectroscopy. We find that stoichiometric surfaces exhibit close to 100% spin polarization at the centre of the surface Brillouin zone at the Fermi edge at ambient temperatures. There is strong evidence for a moment reordering transition at around 80 K which marks the crossover from a high polarization state (T<80 K) to a more representative metallic ferromagnetic state (T>80 K). The results from the different experimental techniques are successively reviewed, with special emphasis on the interplay between composition and electronic structure of the NiMnSb film surfaces. Surface segregation, consistent with a difference in free enthalpy between the surface and the bulk, is induced by annealing treatments. This surface segregation greatly reduces the surface polarization.
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We compare the electronic structure of two metal-centered tetramethyldibenzo-tetraazaannulene (TMTAA) macrocyclic complex molecules: 5,7,12,14- tetramethyl-2,3:9,10-dibenzo[b,i]-1,4,8,11-tetraazacyclotetradecine nickel (II) and 5,7,12,14-tetramethyl-2,3:9,10-dibenzo[b,i]-1,4,8,11-tetraazacyclotetradecine cobalt (II). The experimental gap between the highest occupied molecular orbital to the lowest unoccupied molecular orbital for both molecules, obtained from combined ultraviolet photoemission and inverse photoemission studies, is close to the value of 6.6 eV expected from simple model calculations, but with the Fermi level placed closer to the lowest unoccupied molecular orbital. While both the Co(II) (s = 1/2) and Ni(II) (s = 0) TMTAA molecular electronic structures are very similar, the Ni(II) adopts a high-symmetry molecular configuration upon adsorption, with a strong preferential orientation.
RESUMEN
We compare two mechanisms that dominate the temperature-dependent changes in electronic structure for poly(3-hexylthiophene-2,5 diyl) (P3HT). Structural changes in the relative orientation and configuration of the aromatic ring backbone are observed to occur over a wide range in temperature and affect the local final state screening in photoemission. There are also changes in conductivity and carrier concentration at lower temperatures leading to altered long-range intramolecular screening of photoholes and final state effects that affect excitation spectroscopies including photoemission. For polyethylenedioxythiophene (PEDOT), temperature-dependent changes in the structure and configuration of the polymer backbone are not as significant, although temperature-dependent final state effects are observed.