560 research outputs found
Genuine converging solution of self-consistent field equations for extended many-electron systems
Calculations of the ground state of inhomogeneous many-electron systems
involve a solving of the Poisson equation for Coulomb potential and the
Schroedinger equation for single-particle orbitals. Due to nonlinearity and
complexity this set of equations, one believes in the iterative method for the
solution that should consist in consecutive improvement of the potential and
the electron density until the self-consistency is attained. Though this
approach exists for a long time there are two grave problems accompanying its
implementation to infinitely extended systems. The first of them is related
with the Poisson equation and lies in possible incompatibility of the boundary
conditions for the potential with the electron density distribution. The
analysis of this difficulty and suggested resolution are presented for both
infinite conducting systems in jellium approximation and periodic solids. It
provides the existence of self-consistent solution for the potential at every
iteration step due to realization of a screening effect. The second problem
results from the existence of continuous spectrum of Hamiltonian eigenvalues
for unbounded systems. It needs to have a definition of Hilbert space basis
with eigenfunctions of continuous spectrum as elements, which would be
convenient in numerical applications. The definition of scalar product
specifying the Hilbert space is proposed that incorporates a limiting
transition. It provides self-adjointness of Hamiltonian and, respectively, the
orthogonality of eigenfunctions corresponding to the different eigenvalues. In
addition, it allows to normalize them effectively to delta-function and to
prove in the general case the orthogonality of the 'right' and 'left'
eigenfunctions belonging to twofold degenerate eigenvalues.Comment: 12 pages. Reported on Interdisciplinary Workshop "Nonequilibrium
Green's Functions III", August 22 - 26, 2005, University Kiel, Germany. To be
published in Journal of Physics: Conference Series, 2006; Typos in Eqs. (37),
(53) and (54) are corrected. The content of the footnote is changed.
Published version available free online at
http://www.iop.org/EJ/abstract/1742-6596/35/1/01
The Nature of Electronic States in Atomically Thin MoS2 Field-Effect Transistors
We present low temperature electrical transport experiments in five field
effect transistor devices consisting of monolayer, bilayer and trilayer MoS2
films, mechanically exfoliated onto Si/SiO2 substrate. Our experiments reveal
that the electronic states in all films are localized well up to the room
temperature over the experimentally accessible range of gate voltage. This
manifests in two dimensional (2D) variable range hopping (VRH) at high
temperatures, while below \sim 30 K the conductivity displays oscillatory
structures in gate voltage arising from resonant tunneling at the localized
sites. From the correlation energy (T0) of VRH and gate voltage dependence of
conductivity, we suggest that Coulomb potential from trapped charges in the
substrate are the dominant source of disorder in MoS2 field effect devices,
which leads to carrier localization as well.Comment: 10 pages, 5 figures; ACS Nano (2011
Mechanistic insights into the reversible lithium storage in an open porous carbon via metal cluster formation in all solid-state batteries
Porous carbons are promising anode materials for next generation lithium batteries due to their large lithium storage capacities. However, their high voltage slope during lithiation and delithiation as well as capacity fading due to intense formation of solid electrolyte interphase (SEI) limit their gravimetric and volumetric energy densities. Herein we compare a microporous carbide-derived carbon material (MPC) as promising future anode for all solid-state batteries with a commercial high-performance hard carbon anode. The MPC obtains high and reversible lithiation capacities of 1000 mAh g−1carbon in half-cells exhibiting an extended plateau region near 0 V vs. Li/Li+ preferable for full-cell application. The well-defined micro porosity of the MPC with a specific surface area of >1500 m2 g−1 combines well with the argyrodite-type electrolyte (Li6PS5Cl) suppressing extensive SEI formation to deliver high coulombic efficiencies. Preliminary full-cell measurements vs. nickel-rich NMC-cathodes (LiNi0.9Co0.05Mn0.05O2) provide a considerably improved average potential of 3.76 V leading to a projected energy density as high as 449 Wh kg−1 and reversible cycling for more than 60 cycles. 7Li Nuclear Magnetic Resonance spectroscopy was combined with ex-situ Small Angle X-ray Scattering to elucidate the storage mechanism of lithium inside the carbon matrix. The formation of extended quasi-metallic lithium clusters after electrochemical lithiation was revealed
Fully sp²‐carbon‐linked crystalline two‐dimensional conjugated polymers: insight into 2D poly(phenylenecyanovinylene) formation and their optoelectronic properties
Cyano‐substituted polyphenylene vinylenes (PPVs) have been in the focus of research for several decades due to their interesting optoelectronic properties and potential applications in organic electronics. With the advent of organic two‐dimensional (2D) crystals, the question arose how the chemical and optoelectronic advantages of PPVs evolve in 2D compared to their linear counterparts. In this work, we present the efficent synthesis of two novel 2D fully sp²‐carbon‐linked crystalline PPVs and investigate the essentiality of inorganic bases for their catalytic formation. Notably, among all bases screened, cesium carbonate (Cs₂CO₃) plays a crucial role and enables reversibility in the first step with subsequent structure locking by formation of a C=C double bond to maintain crystallinity, which is supported by density functional theory (DFT) calculation. We propose a quantifiable energy diagram of a “quasi‐reversible reaction” which allows to identify further suitable C‐C bond formation reactions for 2D polymerizations. Moreover, we delineate the narrowing of the HOMO‐LUMO gap by expanding conjugation into two dimensions. To enable environmentally benign processing, we further perform the post‐modification of 2D PPVs, which renders stable dispersions in the aqueous phase
Self-consistent solution of Kohn-Sham equations for infinitely extended systems with inhomogeneous electron gas
The density functional approach in the Kohn-Sham approximation is widely used
to study properties of many-electron systems. Due to the nonlinearity of the
Kohn-Sham equations, the general self-consistence searching method involves
iterations with alternate solving of the Poisson and Schr\"{o}dinger equations.
One of problems of such an approach is that the charge distribution renewed by
means of the Schr\"{o}dinger equation solution does not conform to boundary
conditions of Poisson equation for Coulomb potential. The resulting instability
or even divergence of iterations manifests itself most appreciably in the case
of infinitely extended systems. The published attempts to deal with this
problem are reduced in fact to abandoning the original iterative method and
replacing it with some approximate calculation scheme, which is usually
semi-empirical and does not permit to evaluate the extent of deviation from the
exact solution. In this work, we realize the iterative scheme of solving the
Kohn-Sham equations for extended systems with inhomogeneous electron gas, which
is based on eliminating the long-range character of Coulomb interaction as the
cause of tight coupling between charge distribution and boundary conditions.
The suggested algorithm is employed to calculate energy spectrum,
self-consistent potential, and electrostatic capacitance of the semi-infinite
degenerate electron gas bounded by infinitely high barrier, as well as the work
function and surface energy of simple metals in the jellium model. The
difference between self-consistent Hartree solutions and those taking into
account the exchange-correlation interaction is analyzed. The case study of the
metal-semiconductor tunnel contact shows this method being applied to an
infinitely extended system where the steady-state current can flow.Comment: 38 pages, 9 figures, to be published in ZhETF (J. Exp. Theor. Phys.
Transport properties of copper phthalocyanine based organic electronic devices
Ambipolar charge carrier transport in Copper phthalocyanine (CuPc) is studied
experimentally in field-effect transistors and metal-insulator-semiconductor
diodes at various temperatures. The electronic structure and the transport
properties of CuPc attached to leads are calculated using density functional
theory and scattering theory at the non-equilibrium Green's function level. We
discuss, in particular, the electronic structure of CuPc molecules attached to
gold chains in different geometries to mimic the different experimental setups.
The combined experimental and theoretical analysis explains the dependence of
the mobilityand the transmission coefficient on the charge carrier type
(electrons or holes) and on the contact geometry. We demonstrate the
correspondence between our experimental results on thick films and our
theoretical studies of single molecule contacts. Preliminary results for
fluorinated CuPc are discussed.Comment: 18 pages, 16 figures; to be published in Eur. Phys. J. Special Topic
New mechanism to cross the phantom divide
Recently, type Ia supernovae data appear to support a dark energy whose
equation of state crosses -1, which is a much more amazing problem than the
acceleration of the universe. We show that it is possible for the equation of
state to cross the phantom divide by a scalar field in the gravity with an
additional inverse power-law term of Ricci scalar in the Lagrangian. The
necessary and sufficient condition for a universe in which the dark energy can
cross the phantom divide is obtained. Some analytical solutions with or
are obtained. A minimal coupled scalar with different potentials,
including quadratic, cubic, quantic, exponential and logarithmic potentials are
investigated via numerical methods, respectively. All these potentials lead to
the crossing behavior. We show that it is a robust result which is hardly
dependent on the concrete form of the potential of the scalar.Comment: 11 pages, 5 figs, v3: several references added, to match the
published versio
Structural Mechanism of Laforin Function in Glycogen Dephosphorylation and Lafora Disease
Glycogen is the major mammalian glucose storage cache and is critical for energy homeostasis. Glycogen synthesis in neurons must be tightly controlled due to neuronal sensitivity to perturbations in glycogen metabolism. Lafora disease (LD) is a fatal, congenital, neurodegenerative epilepsy. Mutations in the gene encoding the glycogen phosphatase laforin result in hyperphosphorylated glycogen that forms water-insoluble inclusions called Lafora bodies (LBs). LBs induce neuronal apoptosis and are the causative agent of LD. The mechanism of glycogen dephosphorylation by laforin and dysfunction in LD is unknown. We report the crystal structure of laforin bound to phosphoglucan product, revealing its unique integrated tertiary and quaternary structure. Structure-guided mutagenesis combined with biophysical and biochemical analyses reveal the basis for normal function of laforin in glycogen metabolism. Analyses of LD patient mutations define the mechanism by which subsets of mutations disrupt laforin function. These data provide fundamental insights connecting glycogen metabolism to neurodegenerative disease
Towards analytical typologies of plot systems: quantitative profile of five European cities
The importance of the plot (also referred to as ‘property’) as one of the fundamental elements of urban form is well recognized within the field of urban morphology. Despite the fact that it is often described as the basic element in the pattern of land divisions, which are essential as organizational frameworks for urban form, studies offering comprehensive descriptions and classifications of plot systems are quite scant. The aim of the paper is to introduce a classification of plot systems into typologies based on five European cities, in order to distinguish particular spatial differences and similarities in terms of their plot structure. The proposed typologies are developed using unsupervised k-means cluster analysis based on numeric attributes derived from central theories in urban morphology. The introduced typologies are essentially configurational, allowing collective systematic properties of plot systems to be captured. Numeric attributes include plot differentiation (or plot size), plot frontage and compactness ratio, corresponding to essential qualities of plot systems such as the capacity to carry differences in space, the ability to operate as interface between street and building and providing a framework for evolution of built form over time. All three attributes are translated into configurational measures in order to capture the context of the plot system, rather than the parameters of individual plots. The combination of these deductively defined variables with algorithmically defined classification methods results in seven plot types that can be used to scale up traditional urban morphological analysis to whole city regions and conduct substantial comparison of patterns within, but also between these regions. Further, it also makes it possible to describe commonly recognized plot patterns and discover new ones
- …