Showing papers on "Charge density published in 2007"

Bipolar supercurrent in graphene

Abstract: Graphene--a recently discovered form of graphite only one atomic layer thick--constitutes a new model system in condensed matter physics, because it is the first material in which charge carriers behave as massless chiral relativistic particles. The anomalous quantization of the Hall conductance, which is now understood theoretically, is one of the experimental signatures of the peculiar transport properties of relativistic electrons in graphene. Other unusual phenomena, like the finite conductivity of order 4e(2)/h (where e is the electron charge and h is Planck's constant) at the charge neutrality (or Dirac) point, have come as a surprise and remain to be explained. Here we experimentally study the Josephson effect in mesoscopic junctions consisting of a graphene layer contacted by two closely spaced superconducting electrodes. The charge density in the graphene layer can be controlled by means of a gate electrode. We observe a supercurrent that, depending on the gate voltage, is carried by either electrons in the conduction band or by holes in the valence band. More importantly, we find that not only the normal state conductance of graphene is finite, but also a finite supercurrent can flow at zero charge density. Our observations shed light on the special role of time reversal symmetry in graphene, and demonstrate phase coherent electronic transport at the Dirac point.

Measurement of scattering rate and minimum conductivity in graphene.

Abstract: The conductivity of graphene samples with various levels of disorder is investigated for a set of specimens with mobility in the range of 1-20x10(3) cm2/V sec. Comparing the experimental data with the theoretical transport calculations based on charged impurity scattering, we estimate that the impurity concentration in the samples varies from 2-15x10(11) cm(-2). In the low carrier density limit, the conductivity exhibits values in the range of 2-12e2/h, which can be related to the residual density induced by the inhomogeneous charge distribution in the samples. The shape of the conductivity curves indicates that high mobility samples contain some short-range disorder whereas low mobility samples are dominated by long-range scatterers.

Origin of Charge Density at LaAlO3 on SrTiO3 Heterointerfaces: Possibility of Intrinsic Doping

Abstract: As discovered by Ohtomo and Hwang, a large sheet charge density with high mobility exists at the interface between SrTiO3 and LaAlO3. Based on transport, spectroscopic, and oxygen-annealing experiments, we conclude that extrinsic defects in the form of oxygen vacancies introduced by the pulsed laser deposition process used by all researchers to date to make these samples is the source of the large carrier densities. Annealing experiments show a limiting carrier density. We also present a model that explains the high mobility based on carrier redistribution due to an increased dielectric constant.

Influence of the TiCl4 Treatment on Nanocrystalline TiO2 Films in Dye-Sensitized Solar Cells. 2. Charge Density, Band Edge Shifts, and Quantification of Recombination Losses at Short Circuit

Abstract: Chemical bath deposition of TiO2 from TiCl4 is an often used treatment that improves the photocurrent from dye-sensitized TiO2 solar cells. In this paper, charge density and kinetic data are used to show that the main effects of this treatment are an 80 mV downward shift in the TiO2 conduction band edge potential and a 20-fold decrease in the electron/electrolyte recombination rate constant. Together, these changes increase the quantum efficiency of charge separation at the interface, thus providing the observed increase in the photocurrent. The reduction in the recombination rate constant allows a greater concentration of electrons to accumulate at Voc, thus offsetting the Voc loss otherwise expected from the conduction band edge shift. Photocurrent transients and charge extraction data are used to show that the TiCl4 treatment has little effect on the transport of electrons at short circuit. The electron/electrolyte recombination rate constant at short circuit has been measured with the CCTPV (Constant ...

Ohm's Law at strong coupling: S duality and the cyclotron resonance

Abstract: We calculate the electrical and thermal conductivities and the thermoelectric coefficient of a class of strongly interacting 2+1-dimensional conformal field theories with anti-de Sitter space duals. We obtain these transport coefficients as a function of charge density, background magnetic field, temperature, and frequency. We show that the thermal conductivity and thermoelectric coefficient are determined by the electrical conductivity alone. At small frequency, in the hydrodynamic limit, we are able to provide a number of analytic formulas for the electrical conductivity. A dominant feature of the conductivity is the presence of a cyclotron pole. We show how bulk electromagnetic duality acts on the transport coefficients.

Extension of the Self-Consistent-Charge Density-Functional Tight-Binding Method: Third-Order Expansion of the Density Functional Theory Total Energy and Introduction of a Modified Effective Coulomb Interaction

Abstract: The standard self-consistent-charge density-functional-tight-binding (SCC-DFTB) method (Phys. Rev. B 1998, 58, 7260) is derived by a second-order expansion of the density functional theory total energy expression, followed by an approximation of the charge density fluctuations by charge monopoles and an effective damped Coulomb interaction between the atomic net charges. The central assumptions behind this effective charge−charge interaction are the inverse relation of atomic size and chemical hardness and the use of a fixed chemical hardness parameter independent of the atomic charge state. While these approximations seem to be unproblematic for many covalently bound systems, they are quantitatively insufficient for hydrogen-bonding interactions and (anionic) molecules with localized net charges. Here, we present an extension of the SCC-DFTB method to incorporate third-order terms in the charge density fluctuations, leading to chemical hardness parameters that are dependent on the atomic charge state and...

Charge densities of the neutron and proton

Abstract: A model-independent analysis of the infinite-momentum-frame charge density of partons in the transverse plane is presented for the nucleon We find that the neutron-parton charge density is negative at the center, so that the square of the transverse charge radius is positive, in contrast with many expectations Additionally, the proton's central d quark charge density is larger than that of the u quark by about 30% The proton (neutron) charge density has a long range positively (negatively) charged component

Counterion condensation on charged spheres, cylinders, and planes.

Abstract: We use the framework of counterion condensation theory, in which deviations from linear electrostatics are ascribed to charge renormalization caused by collapse of counterions from the ion atmosphere, to explore the possibility of condensation on charged spheres, cylinders, and planes immersed in dilute solutions of simple salt. In the limit of zero concentration of salt, we obtain Zimm-Le Bret behavior: a sphere condenses none of its counterions regardless of surface charge density, a cylinder with charge density above a threshold value condenses a fraction of its counterions, and a plane of any charge density condenses all of its counterions. The response in dilute but nonzero salt concentrations is different. Spheres, cylinders, and planes all exhibit critical surface charge densities separating a regime of counterion condensation from states with no condensed counterions. The critical charge densities depend on salt concentration, except for the case of a thin cylinder, which exhibits the invariant criticality familiar from polyelectrolyte theory.

Doping and phonon renormalization in carbon nanotubes

Abstract: We show that the Raman frequency associated with the vibrational mode at approximately 1,580 cm(-1) (the G mode) in both metallic and semiconducting carbon nanotubes shifts in response to changes in the charge density induced by an external gate field. These changes in the Raman spectra provide us with a powerful tool for probing local doping in carbon nanotubes in electronic device structures, or charge carrier densities induced by environmental interactions, on a length scale determined by the light diffraction limit. The G mode shifts to higher frequency and narrows in linewidth in metallic carbon nanotubes at large fields. This behaviour is analogous to that observed recently in graphene. In semiconducting carbon nanotubes, on the other hand, induced changes in the charge density only shift the phonon frequency, but do not affect its linewidth. These spectral changes are quantitatively explained by a model that involves the renormalization of the carbon nanotube phonon energy by the electron-phonon interaction as the carrier density in the carbon nanotube is changed.

Effect of field direction on electrowetting in a nanopore

Abstract: We manifest a significant influence of field direction and polarity on surface wetting, when the latter is tuned by application of an external electric field. Thermodynamics of field-induced filling of hydrocarbon-like nanopores with water is studied by open ensemble molecular simulation. Increased field strength consistently results in water-filling and electrostriction in hydrophobic nanopores. A threshold field commensurate with surface charge density of about one elementary charge per 10 nm2 suffices to render prototypical paraffin surfaces hydrophilic. When a field is applied in the direction perpendicular to the confining walls, the competition between orientational polarization and angle preferences of interfacial water molecules relative to the walls results in an asymmetric wettability of opposing surfaces (Janus interface). Reduction of surface free energy observed upon alignment of confinement walls with field direction suggests a novel mechanism whereby the applied electric field can operate s...

Modeling of Surface-Roughness Scattering in Ultrathin-Body SOI MOSFETs

Abstract: A rigorous surface-roughness scattering model for ultrathin-body silicon-on-insulator (SOI) MOSFETs is derived, which reduces to Ando's model in the limit of bulk MOSFETs. The matrix element of the scattering potential reflects the fluctuations of both the wavefunction and the potential energy. The matrix element reflecting the fluctuation of the wavefunction is expressed in an integral form which can be considered as a generalized Prange-Nee term-to which it is equivalent in the limit of an infinitely high insulator-semiconductor barrier-giving more accurate results in the case of a finite barrier height. The matrix element reflecting the fluctuation of the potential energy is due to the Coulomb interactions originating from the roughness-induced fluctuation of the electron charge density, the interface polarization charge, and the image-charge density. The roughness-limited low-field electron mobility in thin-body SOI MOSFETs is obtained using the matrix elements that we have derived. We study its dependence on the silicon body thickness, effective field, and dielectric constant of the insulator.

Charge density of divalent metal cations determines RNA stability

Abstract: RNA molecules are exquisitely sensitive to the properties of counterions. The folding equilibrium of the Tetrahymena ribozyme is measured by nondenaturing gel electrophoresis in the presence of divalent group IIA metal cations. The stability of the folded ribozyme increases with the charge density (ζ) of the cation. Similar scaling is found when the free energy of the RNA folded in small and large metal cations is measured by urea denaturation. Brownian dynamics simulations of a polyelectrolyte show that the experimental observations can be explained by nonspecific ion−RNA interactions in the absence of site-specific metal chelation. The experimental and simulation results establish that RNA stability is largely determined by a combination of counterion charge and the packing efficiency of condensed cations that depends on the excluded volume of the cations.

Charge distribution and screening in layered graphene systems

Abstract: The charge distribution induced by external fields in finite stacks of graphene planes, or in semi-infinite graphite is considered. The interlayer electronic hybridization is described by a nearest-neighbor hopping term, and the charge induced by the self-consistent electrostatic potential is calculated within the linear response theory (random phase approximation). The screening properties are determined by contributions from interband and intraband electronic transitions. In neutral systems, only interband transitions contribute to the charge polarizability, leading to insulatinglike screening properties, and to oscillations in the induced charge, with a period equal to the interlayer spacing. In doped systems, we find a screening length that is equivalent to two-to-three graphene layers, superimposed to significant charge oscillations.

Nuclear Charge Radius of He 8

Abstract: The root-mean-square (rms) nuclear charge radius of $^{8}\mathrm{He}$, the most neutron-rich of all particle-stable nuclei, has been determined for the first time to be 1.93(3) fm. In addition, the rms charge radius of $^{6}\mathrm{He}$ was measured to be 2.068(11) fm, in excellent agreement with a previous result. The significant reduction in charge radius from $^{6}\mathrm{He}$ to $^{8}\mathrm{He}$ is an indication of the change in the correlations of the excess neutrons and is consistent with the $^{8}\mathrm{He}$ neutron halo structure. The experiment was based on laser spectroscopy of individual helium atoms cooled and confined in a magneto-optical trap. Charge radii were extracted from the measured isotope shifts with the help of precision atomic theory calculations.

Charge Ordering in α-(BEDT-TTF)2I3 by Synchrotron X-ray Diffraction

Abstract: The spatial charge arrangement of a typical quasi-two-dimensional organic conductor α-(BEDT-TTF) 2 I 3 is revealed by single crystal structure analysis using synchrotron radiation. The results show that the horizontal-stripe-type structure, which was suggested by the mean field theory, is established. We also find the charge disproportionation above the metal–insulator transition temperature and a significant change in the transfer integrals caused by the phase transition. Our result elucidates the insulating phase of this material as the 2 k F charge density localization.

Geometry, charge distribution, and surface speciation of phosphate on goethite.

Abstract: The surface speciation of phosphate has been evaluated with surface complexation modeling using an interfacial charge distribution (CD) approach based on ion adsorption and ordering of interfacial water. In the CD model, the charge of adsorbed ions is distributed over two electrostatic potentials in the double-layer profile. The CD is related to the structure of the surface complex. A new approach is followed in which the CD values of the various surface complexes have been calculated theoretically from the geometries of the surface complexes. Molecular orbital calculations based on density functional theory (MO/DFT) have been used to optimize the structure of a series of hydrated surface complexes of phosphate. These theoretical CD values are corrected for dipole orientation effects. Data analysis of the PO4 adsorption, applying the independently derived CD coefficients, resolves the presence of two dominant surface species. A nonprotonated bidentate (B) complex is dominant over a broad range of pH values at low loading (1.5 mol/m2). For low pH and high loading, a strong contribution of a singly protonated monodentate (MH or MH-Na) complex is found, which differs from earlier interpretations. For the conditions studied, the doubly protonated bidentate (BH2) and monodentate (MH2) surface complexes and the nonprotonated monodentate (M) complex are not significant contributors. These findings are discussed qualitatively and quantitatively in relation to published experimental in-situ CIR-FTIR data and theoretical MO/DFT-IR information. The relative variation in the peak intensities as a function of pH and loading approximately agrees with the surface speciation calculated with the CD model. The model correctly predicts the proton co-adsorption of phosphate binding on goethite and the shift of the IEP at low phosphate loading (1.5 mol/m2). At higher loading, it deviates.

Gate coupling and charge distribution in nanowire field effect transistors.

Abstract: We have modeled the field and space charge distributions in back-gate and top-gate nanowire field effect transistors by solving the three-dimensional Poisson's equation numerically. It is found that the geometry of the gate oxide, the semiconductivity of the nanowire, and the finite length of the device profoundly affect both the total amount and the spatial distribution of induced charges in the nanowire, in stark contrast to the commonly accepted picture where metallic dielectric properties and infinite length are assumed for the nanowire and the specific geometry of the gate oxide is neglected. We provide a comprehensive set of numerical correction factors to the analytical capacitance formulas, as well as to numerical calculations that neglect the semiconductivity and finite length of the nanowire, that are frequently used for quantifying carrier transport in nanowire field effect transistors.

Self-consistency over the charge density in dynamical mean-field theory: A linear muffin-tin implementation and some physical implications

Abstract: We present a simple implementation of the dynamical mean-field-theory approach to the electronic structure of strongly correlated materials. This implementation achieves full self-consistency over the charge density, taking into account correlation-induced changes to the total charge density and effective Kohn-Sham Hamiltonian. A linear muffin-tin orbital basis set is used, and the charge density is computed from moments of the many-body momentum-distribution matrix. The calculation of the total energy is also considered, with a proper treatment of high-frequency tails of the Green's function and self-energy. The method is illustrated on two materials with well-localized $4f$ electrons, insulating cerium sesquioxide ${\mathrm{Ce}}_{2}{\mathrm{O}}_{3}$ and the $\ensuremath{\gamma}$ phase of metallic cerium, using the Hubbard-I approximation to the dynamical mean-field self-energy. The momentum-integrated spectral function and momentum-resolved dispersion of the Hubbard bands are calculated, as well as the volume dependence of the total energy. We show that full self-consistency over the charge density, taking into account its modification by strong correlations, can be important for the computation of both thermodynamical and spectral properties, particularly in the case of the oxide material.

Polarization Relaxation in an Ionic Liquid Confined between Electrified Walls

Abstract: The response of a room temperature molten salt to an external electric field when it is confined to a nanoslit is studied by molecular dynamics simulations. The fluid is confined between two parallel and oppositely charged walls, emulating two electrified solid-liquid interfaces. Attention is focused on structural, electrostatic, and dynamical properties, which are compared with those of the nonpolarized fluid. It is found that the relaxation of the electrostatic potential, after switching the electric field off, occurs in two stages. A first, subpicosecond process accounts for 80% of the decay and is followed by a second subdiffusive process with a time constant of 8 ps. Diffusion is not involved in the relaxation, which is mostly driven by small anion translations. The relaxation of the polarization in the confined system is discussed in terms of the spectrum of charge density fluctuations in the bulk.

Thermodiffusion of charged colloids: single-particle diffusion.

Abstract: An expression for the single-particle thermal diffusion coefficient of a charged colloidal sphere is derived on the basis of force balance on the Brownian time scale in combination with thermodynamics. It is shown that the single-particle thermal diffusion coefficient is related to the temperature dependence of the reversible work necessary to build the colloidal particle, including the core, the solvation layer, and the electrical double layer. From this general expression, an explicit expression for the contribution of the electrical double layer to the single-particle thermal diffusion coefficient is derived in terms of the surface charge density of the colloidal sphere, the electrostatic screening length, and its core radius, to within the Debye-Huckel approximation. This result is shown to explain experimental data, for both thin and thick double layers. In addition, a comparison with other theories is made.

Charge Ordering in alpha-(BEDT-TTF)2I3 by synchrotron x-ray diffraction

Abstract: The spatial charge arrangement of a typical quasi-two-dimensional organic conductor alpha-(BEDT-TTF)2I3 is revealed by single crystal structure analysis using synchrotron radiation. The results show that the horizontal stripe type structure, which was suggested by mean field theory, is established. We also find the charge disproportion above the metal-insulator transition temperature and a significant change in transfer integrals caused by the phase transition. Our result elucidates the insulating phase of this material as a 2k_F charge density localization.

Electrohydrodynamic flow around a colloidal particle near an electrode with an oscillating potential

Abstract: Electrohydrodynamic (EHD) flow around a charged spherical colloid near an electrode was studied theoretically and experimentally to understand the nature of long-range particle–particle attraction near electrodes. Numerical computations for finite double-layer thicknesses confirmed the validity of an asymptotic methodology for thin layers. Then the electric potential around the particle was computed analytically in the limit of zero Peclet number and thin double layers for oscillatory electric fields at frequencies where Faradaic reactions are negligible. Streamfunctions for the steady component of the EHD flow were determined with an electro-osmotic slip boundary condition on the electrode surface. Accordingly, it was established how the axisymmetric flow along the electrode is related to the dipole coefficient of the colloidal particle. Under certain conditions, the flow is directed toward the particle and decays as r−4, in accord with observations of long-range particle aggregation. To test the theory, particle-tracking experiments were performed with fluorescent 300 nm particles around 50μm particles over a wide range of electric field strengths and frequencies. Treating the particle surface conductivity as a fitting parameter yields velocities in excellent agreement with the theoretical predictions. The observed frequency dependence, however, differs from the model predictions, suggesting that the effect of convection on the charge distribution is not negligible as assumed in the zero Peclet number limit.

Conformational adaptation and selective adatom capturing of tetrapyridyl-porphyrin molecules on a copper (111) surface

Abstract: We present a combined low-temperature scanning tunneling microscopy and near-edge X-ray adsorption fine structure study on the interaction of tetrapyridyl-porphyrin (TPyP) molecules with a Cu(111) surface. A novel approach using data from complementary experimental techniques and charge density calculations allows us to determine the adsorption geometry of TPyP on Cu(111). The molecules are centered on “bridge” sites of the substrate lattice and exhibit a strong deformation involving a saddle-shaped macrocycle distortion as well as considerable rotation and tilting of the meso-substituents. We propose a bonding mechanism based on the pyridyl−surface interaction, which mediates the molecular deformation upon adsorption. Accordingly, a functionalization by pyridyl groups opens up pathways to control the anchoring of large organic molecules on metal surfaces and tune their conformational state. Furthermore, we demonstrate that the affinity of the terminal groups for metal centers permits the selective captur...