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At least 1,171 records · Page 65

Many-body Green's function approaches to the doped Fröhlich solid: Exact solutions and anomalous mass enhancement

In polar semiconductors and insulators, the Fröhlich interaction between electrons and long-wavelength longitudinal optical phonons induces a many-body renormalization of the carrier effective masses and the appearance of characteristic phonon sidebands in the spectral function, commonly dubbed “polaron satellites.” The simplest model that captures these effects is the Fröhlich model, whereby electrons in a parabolic band interact with a dispersionless longitudinal optical phonon. The Fröhlich model has been employed in a number of seminal papers, from early perturbation-theory approaches to modern diagrammatic Monte Carlo calculations. One limitation of this model is that it focuses on undoped systems, thus ignoring carrier screening and Pauli blocking effects that are present in real experiments on doped samples. Here, to overcome this limitation, we extend the Fröhlich model to the case of doped systems, and we provide exact solutions for the electron spectral function, mass enhancement, and polaron satellites. We perform the analysis using two approaches, namely, Dyson’s equation with the Fan-Migdal self-energy, and the second-order cumulant expansion. We find that these two approaches provide qualitatively different results. In particular, Dyson’s approach yields better quasiparticle masses and worse satellites, while the cumulant approach provides better satellite structures, at the price of worse quasiparticle masses. Both approaches yield an anomalous enhancement of the electron effective mass at finite doping levels, which in turn leads to a breakdown of the quasiparticle picture in a significant portion of the phase diagram.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetic quantum phase transition in Cr-doped Bi 2 (Se x Te 1-x ) 3 driven by the Stark effect

The interplay between magnetism and topology, as exemplified in the magnetic skyrmion systems, has emerged as a rich playground for finding novel quantum phenomena and applications in future information technology. Magnetic topological insulators (TI) have attracted much recent attention, especially after the experimental realization of quantum anomalous Hall effect. Future applications of magnetic TI hinge on the accurate manipulation of magnetism and topology by external perturbations, preferably with a gate electric field. In this work, we investigate the magneto transport properties of Cr doped Bi 2 (Se x Te 1-x ) 3 TI across the topological quantum critical point (QCP). We find that the external gate voltage has negligible effect on the magnetic order for samples far away from the topological QCP. However, for the sample near the QCP, we observe a ferromagnetic (FM) to paramagnetic (PM) phase transition driven by the gate electric field. Theoretical calculations show that a perpendicular electric field causes a shift of electronic energy levels due to the Stark effect, which induces a topological quantum phase transition and consequently a magnetic phase transition. Finally, the in situ electrical control of the topological and magnetic properties of TI shed important new lights on future topological electronic or spintronic device applications.

36 MATERIALS SCIENCE↗

Electrospun ZnO Nanoparticles Doped Core–Sheath Nanofibers: Characterization and Antimicrobial Properties

Coaxial electrospinning technique was used to fabricate the core–sheath composite nanofibers of ZnO nanoparticle (Nps) (10%, 20% w/w) doped polymethyl methacrylate (PMMA) (as sheath) and polyvinyl alcohol (PVA) (as core). Fourier transform infrared (FT-IR) spectra were confirmed the weak forces arise between ZnO Nps, PMMA and PVA matrixes. The hexagonal (wurtzite) structure of ZnO Nps with ~ 30.8 nm of diameter was confirmed from the X-ray diffraction pattern. The morphology and microstructure of core–sheath composite nanofibers were confirmed from the scanning electron microscopy (SEM) and transmission electron microscopy (TEM). It is clearly seen from the TEM images that the PMMA encapsulate the PVA core. Core–sheath composite nanofibers were assessed against Escherichia coli (E. coli) and Bacillus subtilis (B. subtilis) bacteria through quantitative, disk diffusion and viable cell count methods. It was found that ZnO Nps doped core–sheath nanofibers were effectively inhibit the growth of gram positive bacteria, B. subtilis.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

The photocatalytic performance of Ta and Rh co-doped TiO2 tuned by the average dopant valence

Highlights: • Effects of dopant valence on the photocatalytic performance was investigated. • New strategy was worked out to investigate effects of dopant valence. • The dopant valence was changed but the ionic radius keeps constant. • Average valence of Rh and Ta in Ti{sub 0.96}Ta{sub 0.04−x}Rh{sub x}O{sub 2} was changed multiply. • The optimal photocatalyst was obtained as the average valence approaches +4. - Abstract: In order to reveal the effects of dopant average valence on the photocatalytic performance, Ta and Rh co-doped Ti{sub 0.96}Ta{sub 0.04−x}Rh{sub x}O{sub 2} (x = 0, 0.008, 0.016, 0.02, 0.024, 0.032, and 0.04) samples were crystallized at 450 °C and 800 °C, respectively; then the 800 °C crystallized x = 0.02 sample was subsequently reduced in the H{sub 2}/N{sub 2} mixture gases at 600, 700, 800, and 900 °C. Under different processing conditions, Ta remains the valence of +5, while the valence of Rh varies. Rh exhibits Rh{sup 3+} and Rh{sup 4+} in the 450 °C crystallized samples and is completely oxidized to Rh{sup 4+} in the 800 °C crystallized samples. In the reduced samples, Rh exists in the forms of Rh, Rh{sup 3+} and Rh{sup 4+}. The optimal photocatalyst is obtained as the ratio of Rh{sup 3+}/Rh{sup 4+} is 2.11 or the average valence of doped Ta and Rh is closest to the +4 valence of substituted Ti.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Divalent doping-induced thermoelectric power factor increase in p-type Bi 2 Te 3 via electronic structure tuning

We use first-principles calculations to reveal the effects of divalent Pb, Ca, and Sn doping of Bi 2 Te 3 on the band structure and transport properties, including the Seebeck coefficient, α, and the reduced power factor, α 2 σ/τ, where σ is the electrical conductivity and τ is the effective relaxation time. Pb and Ca additions exhibit up to 60%–75% higher peak α 2 σ/τ than that of intrinsic Bi 2 Te 3 with Bi antisite defects. Pb occupancy and Ca occupancy of Bi sites increase σ/τ by activating high-degeneracy low-effective-mass bands near the valence band edge, unlike Bi antisite occupancy of Te sites that eliminates near-edge valence states in intrinsic Bi 2 Te 3 . Neither Pb doping nor subatomic-percent Ca doping increases α significantly, due to band averaging. Higher Ca levels increase α and diminish σ, due to the emergence of a corrugated band structure underpinned by high-effective-mass bands, attributable to Ca–Te bond ionicity. Sn doping results in a distortion of the bands with a higher density of states that may be characterized as a resonant state but decreases α 2 σ by up to 30% due to increases in the charge carrier effective mass and decreases in both spin–orbit coupling and valence band quasidegeneracy. These results, and thermal conductivity calculations for nanostructured Bi 2 Te 3 , suggest that Pb or Ca doping can enhance the thermoelectric figure of merit ZT to values up to ZT ~ 1.7, based on an experimentally determined τ. Our findings suggest that divalent doping can be attractive for realizing large ZT enhancements in pnictogen chalcogenides.

36 MATERIALS SCIENCE↗

Scanning Kelvin Probe Microscopy: A Tool to Investigate Nano-Scale Doping Non-Uniformities in Poly-Si/SiOx Contacts: Preprint

Monocrystalline Si (c-Si) solar cells with passivated contacts based on the ultrathin SiOx and doped polycrystalline Si (poly-Si) layers in a poly-Si/SiOx/c Si structure show high solar cell efficiencies that are ~26%. Excellent surface passivation using these contacts is achieved via the combined effects of chemical passivation of the SiOx/c-Si interface by the SiOx layer and field-effect passivation from the heavily doped poly-Si layer. These contacts give best performance only when annealed to temperatures higher than 850 degrees C. Structural changes in the SiOx layer and dopant diffusion from poly-Si into the underlying c-Si wafer occur during this step which are hard to investigate using conventional characterization techniques. In this work we investigate poly-Si/SiOx contacts with both a 1.5 (tunneling transport) and 2.2 (pinhole transport) nm SiOx layer using atomic force microscopy techniques. Conductive AFM on n+-poly-Si/SiOx/p-Si structures show significant spatial variations for both contact types, likely due to non-uniformities in the poly-Si layer itself. The electrical and structural variations deeper into the contact were revealed by scanning Kelvin probe microscopy after precisely etching away the poly-Si and SiOx layers and few nanometers of c-Si surface. This etching was performed using tetramethylammonium hydroxide and dilute HF solutions. The resulting surface potential maps appear similar for both contacts, and show less than 500 nm size heavily-doped regions. However, further etching of the c-Si surface reveals these heavily-doped regions to be less than 200 nm deep for the 2.2 nm SiOx contact and greater than 200 nm deep for the 1.5 nm SiOx contact.

14 SOLAR ENERGY↗

Two-dimensional superconductor-insulator quantum phase transitions in an electron-doped cuprate

Here, we use an ionic liquid-assisted electric-field effect to tune the carrier density in an electron-doped cuprate ultrathin film and cause a two-dimensional superconductor-insulator transition (SIT). The low upper critical field in this system allows us to perform magnetic-field (B)-induced SIT in the liquid-gated superconducting film. Finite-size scaling analysis indicates that SITs induced both by electric and by magnetic fields are quantum phase transitions and the transitions are governed by percolation effects-quantum mechanical in the former and classical in the latter cases. Compared to the hole-doped cuprates, the SITs in the electron-doped system occur at critical sheet resistances (R c ) much lower than the pair quantum resistance R Q = h/(2e) 2 = 6.45 kΩ, suggesting the possible existence of fermionic excitations at finite temperatures at the insulating phase near the SITs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Structural, magnetic, and transport properties of Fe-doped CoTiSb epitaxial thin films

Epitaxial intrinsic and Fe-doped CoTiSb thin films with C1{sub b} structure were grown on MgO(100) substrates by magnetron sputtering. The semiconducting-like behavior in both intrinsic and Fe-doped thin films was demonstrated by temperature dependence of longitudinal resistivity. The Fe-doped CoTiSb films with a wide range of doping concentrations can maintain semiconducting-like and magnetic properties simultaneously, while the semiconducting behavior is weakening with the increasing Fe concentration. For 21 at. % Fe-doped film, low lattice magnetic moment (around 0.65 μ{sub B}) and high resistivity (larger than 800 μΩ cm) are beneficial to its application as a magnetic electrode in spintronic devices. Anomalous Hall effect of 21 at. % Fe-doped film was also investigated and its behaviors can be treated well by recent-reported anomalous Hall scaling including the contribution of spin-phonon skew scattering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Rare Earth and Transition Metal Containing Glasses

Transition metal (TM) and rare earth (RE) ions have been incorporated into many glass systems such as silicate, phosphate, and borosilicate-based oxide glasses, as well as in halide and chalcogenide glasses, that find applications ranging from optical, photonic, and magnetic devices, solid-state battery, to nuclear waste disposal. Understanding the structural role of RE and TM in these glasses can help to develop glass compositions for targeted applications with either high-optical emission efficiency, electrical conductivity, or chemical durability. In this chapter, we first provide a general introduction of the applications and structural features of RE and TM in glasses, then the critical aspects of molecular dynamics (MD) simulations of these glasses such as interatomic potentials, structural analysis tools to study RE and TM ions in glasses and their clustering behaviors, Quantitative Structure–Property Analysis (QSPR), diffusion and dynamic property calculations, and electronic structure calculations to understand electronic defects such as charge trapping and radiation effects are introduced. Three representative case studies are presented: the first one is on MD simulations of erbium- and europium-doped silica and silicate glasses, as well as cerium doped aluminophosphate glasses, that revealed the effect of glass composition on RE ion local structure and clustering behavior. Electronic structure calculations of cerium-doped glass show how the existence of multioxidation states help to mediate radiation-induced damages caused by excited electron–hole pairs was also discussed. The second one focuses on alkali vanadophosphate glasses where the existence of two vanadium oxidation states help to provide electronic conduction in the glasses while alkali ions provide ionic conduction. MD simulations were used to understand vanadium environments and other structural aspects in the phosphate glasses, as well as the ionic transport behaviors of alkali ions. The third case study is on zirconium-containing borosilicate and aluminosilicate glasses that find wide applications in nuclear waste disposal. MD simulations help to provide structural details of zirconium ions that are validated by diffraction and EXAFS spectra. The structural information was used to interpret changes of mechanical properties and chemical durability by using QSPR and other analyses-based MD-generated structure models.

Du, Jincheng↗

Li doped kagome spin liquid compounds

We elucidate the unexpected insulating features of Li-doped QSL compounds by proposing a charge localization effect due to chemical bonding.

Chemistry↗

Surface Charge and Electrostatic Spin Crossover Effects in CoN 4 Electrocatalysts

Carbon materials doped with nitrogen and 3d transition metals have attracted a great deal of interest for catalyzing electrochemical reactions such as water splitting, oxygen reduction, and carbon dioxide reduction. Here, we employed density functional theory to study Co–N-doped carbon as electrocatalysts for the oxygen reduction and oxygen evolution reactions. Specifically, we investigated the interplay among adsorption energies, the spin state of the CoN 4 active center, and the applied potential. We found that adsorption energies strongly depend on both the applied potential and the spin state of the Co center. Furthermore, spin state transitions induced by the applied potential also play an important role in determining the adsorption energies. Here, this effect originates from a different potential of zero charge and capacitance of each spin state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of Oxygen Vacancy on the Magnetic Properties of Ni-Doped SnO{sub 2} Nanoparticles

We studied the ferromagnetism of Ni-doped SnO{sub 2} with and without oxygen vacancy (V{sub O}) by experiments and calculations. Sn{sub 0.96}Ni{sub 0.04}O{sub 2} nanocrystalline powder prepared by the sol-gel method exhibits room-temperature ferromagnetism, and the vacuum annealing reduces its saturation magnetizations. The density functional theory (DFT) calculations show that the doped Ni atom can introduce a local magnetic moment of about 2.0 μ{sub B} in SnO{sub 2} (110) surface, which is ascribed to the spin-polarization of Ni 3d and O 2p electrons. The type of preferential magnetic coupling of Ni-doped SnO{sub 2} (110) surface depends upon the distributions of Ni dopants, and ferromagnetic coupling is more favorable in most cases. Introduction of V{sub O} obviously weakens the ferromagnetic interaction of Ni-doped SnO{sub 2} (110) surface, which can give a reasonable explanation for our experimental observations.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Effect of high temperature annealing on the thermoelectric properties of GaP doped SiGe

Silicon-germanium alloys doped with GaP are used for thermoelectric energy conversion in the temperature range 300-1000 C. The conversion efficiency depends on Z = S-squared/rho lambda, a material's parameter (the figure of merit), where S is the Seebeck coefficient, rho is the electrical resistivity and lambda is the thermal conductivity. The annealing of several samples in the temperature range of 1100-1300 C resulted in the power factor P (= S-squared/rho) increasing with increased annealing temperature. This increase in P was due to a decrease in rho which was not completely offset by a drop in S-squared suggesting that other changes besides that in the carrier concentration took place. SEM and EDX analysis of the samples indicated the formation of a Ga-P-Ge rich phase as a result of the annealing. It is speculated that this phase is associated with the improved properties. Several reasons which could account for the improvement in the power factor of annealed GaP doped SiGe are given.

Vandersande, Jan W.↗

Doping directed at the oxygen sites in Y1Ba2Cu3O(7-delta) - The effect of sulfur, fluorine, and chlorine

The effect of three dopants directed at the oxygen sites in Y1Ba2Cu3O(7-delta) have been investigated: sulfur, fluorine, and chlorine. Single-phase material has been obtained up to a (nominal) replacement of about 1 percent of the oxygen. Although the lattice parameters are unchanged, all dopants raise Tc (very slightly), sharpen the resistive transition, reduce the normal state resistivity, and very substantially increase the (magnetically determined) fraction of the material that is superconducting. All of these results differ qualitatively from those obtained with dopants directed at other locations in the 123 structure, and it is suggested that small additions of sulfur, fluorine, or chlorine may help to stabilize the ideal 123 stoichiometry.

Bansal, N. P.↗

Al-doped ZnO seed layer-dependent crystallographic control of ZnO nanorods by using electrochemical deposition

Highlights: • Polar and semipolar ZnO NRs were successfully achieved by hydrothermal synthesis. • Semipolar and polar ZnO NRs were grown on ZnO and AZO/m-sapphire, respectively. • Al % of AZO/m-sapphire enhanced the lateral growth rate of polar ZnO NRs. - Abstract: We investigated the effect of an Al-doped ZnO film on the crystallographic direction of ZnO nanorods (NRs) using electrochemical deposition. From high-solution X-ray diffraction measurements, the crystallographic plane of ZnO NRs grown on (1 0 0) ZnO/m-plane sapphire was (1 0 1). The surface grain size of the (100) Al-doped ZnO (AZO) film decreased with increasing Al content in the ZnO seed layer, implying that the Al dopant accelerated the three-dimensional (3D) growth of the AZO film. In addition, it was found that with increasing Al doping concentration of the AZO seed layer, the crystal orientation of the ZnO NRs grown on the AZO seed layer changed from [1 0 1] to [0 0 1]. With increasing Al content of the nonpolar (1 0 0) AZO seed layer, the small surface grains with a few crystallographic planes of the AZO film changed from semipolar (1 0 1) ZnO NRs to polar (0 0 1) ZnO NRs due to the increase of the vertical [0 0 1] growth rate of the ZnO NRs owing to excellent electrical properties.

36 MATERIALS SCIENCE↗