Tuning of energy levels and optical properties of graphene quantum dots

We investigate theoretically the magnetic levels and optical properties of zigzag- and armchair-edged hexagonal graphene quantum dots (GQDs) utilizing the tight-binding method. A bound edge state at zero energy appears for the zigzag GQDs in the absence of a magnetic field. The magnetic levels of GQDs exhibit a Hofstadter-butterfly spectrum and approach the Landau levels of two-dimensional graphene as the magnetic field increases. The optical properties are tuned by the size, the type of the edge, and the external magnetic field.

Spin-Hall effect in the generalized honeycomb lattice with Rashba spin-orbit interaction

We study the spin-Hall effect in a generalized honeycomb lattice, which is described by a tight-binding Hamiltonian including the Rashba spin-orbit coupling and inversion-symmetry breaking terms brought about by a uniaxial pressure. The calculated spin-Hall conductance displays a series of exact or approximate plateaus for isotropic or anisotropic hopping integral parameters, respectively. We show that these plateaus are a consequence of the various Fermi-surface topologies when tuning epsilon(F). For the isotropic case, a consistent two-band analysis, as well as a Berry-phase interpretation. are also given. (C) 2009 Elsevier B.V. All rights reserved.

A partially incoherent rate theory of long-range charge transfer in deoxyribose nucleic acid

A quantum chemistry based Green's function formulation of long-range charge transfer in deoxyribose nucleic acid (DNA) double helix is proposed. The theory takes into account the effects of DNA's electronic structure and its incoherent interaction with aqueous surroundings. In the implementation, the electronic tight-binding parameters for unsolvated DNA molecules are determined at the HF/6-31G* level, while those for individual nucleobase-water couplings are at a semiempirical level by fitting with experimental redox potentials. Numerical results include that: (i) the oxidative charge initially at the donor guanine site does hop sequentially over all guanine sites; however, the revealed rates can be of a much weaker distance dependence than that described by the ordinary Ohm's law; (ii) the aqueous surroundings-induced partial incoherences in thymine/adenine bridge bases lead them to deviate substantially from the superexchange regime; (iii) the time scale of the partially incoherent hole transport through the thymine/adenine pi stack in DNA is about 5 ps. (C) 2002 American Institute of Physics.

In-plane optical anisotropy in asymmetric Si1-xGex/Si/Si1-yGey superlattices

A trilayer asymmetric superlattice, Si/Si1-xGex/Si1-yGey, is proposed, in which the broken inversion symmetry makes the microstructure optically biaxial; in particular, inequivalent interfaces in this heterostructure may cause a polarization ratio as large as about 2.5% in the absence of an external field. The electronic structure and absorption spectra for two types of trilayer superlattice with different parameters are calculated by use of the tight-binding model; the findings indicate the importance of the carrier confinement for the anisotropy value. The effect of external electric field on the optical anisotropy for such structures has also been discussed, and a Pockels coefficient of 10-9 cm V-1 estimated.

SELF-CONSISTENT TREATMENT OF 3-DIMENSIONAL - 2-DIMENSIONAL AND 2-DIMENSIONAL - 2-DIMENSIONAL RESONANT-TUNNELING IN DOUBLE-BARRIER STRUCTURES

By using a transfer-matrix method on the basis of two-dimensional (2D) Bloch sums in accordance with a tight-binding scheme, a self-consistent calculation on the resonant tunneling in asymmetric double-barrier structures is presented, in which contributions to resonant tunneling from both three-dimensional (3D) electrons in the contacts and 2D electrons in the spacer or accumulation layers are considered simultaneously. The charge buildup effect on the current versus voltage (I-V) curves is evaluated systematically, showing quantitatively how it results in the I-V bistability and enhanced differences between I-V curves for positive and negative bias in an asymmetric double-barrier structure. Special attention is focused on the interaction between 3D-2D and 2D-2D resonant-tunneling processes, including the suppression of 2D-2D resonant tunneling by the charge buildup in the well accompanying the 3D-2D resonant tunneling. The effects of the emitter doping condition (doping concentration, spacer thickness) on the presence of two types of quasi-2D levels in the emitter accumulation layers, and on the formation of a potential bulge in the emitter region, are discussed in detail in relation to the tunneling process.

OXYGEN IN INXGA1-XASYP1-Y GROWN ON GAAS

The measurement of DLTS on the alloy InxGa1-xAsyP1-y (0 less-than-or-equal-to y less-than-or-equal-to 0.3; 0.5 greater-than-or-equal-to x greater-than-or-equal-to 0.35) shows a new signal, labeled as E2, with an activation energy of E(c) - 0.61 eV and the SIMS signals show a large number of oxygen. To clarify is further, the energy of the deep level E2 is quantitatively calculated by using Vogl's tight-binding theory and Hjalmarson's deep level theory. As a result, the deep A1-symmetric level associated with an oxygen on the anion site of InxGa1-xAsyP1-y locates deeply in the band gap. Thus, the level E2 is considered to be induced by the oxygen impurity.

BAND DISPERSION IN THE RECURSION METHOD

The advantages of the supercell model in employing the recursion method are discussed in comparison with the cluster model. A transformation for changing complex Bloch-sum seed states to real seed states in recursion calculations is presented and band dispersion in the recursion method is extracted with use of the Lanczos algorithm. The method is illustrated by the band structure of GaAs in the empirical tight-binding parametrized model. In the supercell model, the treatment of boundary conditions is discussed for various seed-state choices. The method is useful in applying tight-binding techniques to systems with substantial deviations from periodicity.

Suppression of ballistic electron transmission through a semiconductor II-structure by an external transverse electric field

We have conducted numerical studies of ballistic electron transport in a semiconductor II-structure when an external transverse electric field is applied. The device conductance as a function of electron energy and the strength of the transverse electric field is calculated on the basis of tight-binding Green's function formalism. The calculations show that a relatively weak electric field can induce very large decrease in the electron transmission across the structure. When the transverse electric field is sufficiently strong, electrons can hardly be transported through the device. Thus the performance of the device can be greatly improved for it is much easier to control electron transport through the device with an external transverse electric field.

基于紧束缚分子动力学模型的Na4,Na8和Na20团簇结构及热力学性质研究

利用距离相关的紧束缚的分子动力学模型（DDTB－MD），通过提取不同温度下的势能、构型、无单位键长涨落平均位移、扩散系数、围绕质心的径向分布等参量，系统的研究了菱形结构和T形结构的Na4、Td结构和D2d结构的Na8，以及Na20的热力学的性质。对于Na4，比较了金属团簇Na4的菱形结构和T形结构两种异构体之间热力学性质的异同。发现在团簇温度升高的过程中，两种异构体都会发生从类固到类液的相变。T形结构的Na4熔点要比菱形结构的低。在相变的过程中都会发生赝转动和异构化。还发现了赝转动的判据不仅仅只是温度，还包括无单位键长涨落的δ值。菱形结构的Na4在200K左右不一定会发生赝转动，只有观察到温度处于200K左右，δ值≥0.08的时候，赝转动则必然会观察到。菱形结构Na4的赝转动过程中会发现T形结构的异构化，但其维持时间很短，不稳定，很快又转变为菱形结构。而T形结构在170K就能观察到异构化和赝转动的发生，在这个温度下会不断的在菱形与T型之间发生异构，而处于菱形结构的时间要比T型长的多。表现为菱形结构的稳定性要大于T型。对于Na8的两种不同的异构体（分别为Td结构和D2d结构），发现尽管两个异构体的基态能量很接近，但他们的稳定性、熔化过程的热力学性质等有着很大的差别，这也反映了它们在几何结构上的差别。对称性强的Td结构更紧密，在熔化过程中表现出更高的稳定性，具有较高的熔点，具有类晶体的性质.对称性弱的D2d结构则具有较低的熔点，很宽的熔化温度范围，具有类似非晶体的性质. 再比较了基态结构下的Na8和Na20。通过提取对不同的子系统在不同温度下的无单位键长涨落等参数，发现金属原子团簇Na20在熔化过程中表现出了并不像通常金属团簇那样的表面先熔化，而是从内部开始先熔化的奇异特性

Theory of the electronic and optical properties of dilute bismide alloys

Dilute bismide alloys, containing small fractions of bismuth (Bi), have recently attracted interest due to their potential for applications in a range of semiconductor devices. Experiments have revealed that dilute bismide alloys such as GaBixAs1−x, in which a small fraction x of the atoms in the III-V semiconductor GaAs are replaced by Bi, exhibit a number of unusual and unique properties. For example, the band gap energy (E g) decreases rapidly with increasing Bi composition x, by up to 90 meV per % Bi replacing As in the alloy. This band gap reduction is accompanied by a strong increase in the spin-orbit-splitting energy (ΔSO) with increasing x, and both E g and ΔSO are characterised by strong, composition-dependent bowing. The existence of a ΔSO > E g regime in the GaBixAs1−x alloy has been demonstrated for x ≳10%, a band structure condition which is promising for the development of highly efficient, temperature stable semiconductor lasers that could lead to large energy savings in future optical communication networks. In addition to their potential for specific applications, dilute bismide alloys have also attracted interest from a fundamental perspective due to their unique properties. In this thesis we develop the theory of the electronic and optical properties of dilute bismide alloys. By adopting a multi-scale approach encompassing atomistic calculations of the electronic structure using the semi-empirical tight-binding method, as well as continuum calculations based on the k•p method, we develop a fundamental understanding of this unusual class of semiconductor alloys and identify general material properties which are promising for applications in semiconductor optoelectronic and photovoltaic devices. By performing detailed supercell calculations on both ordered and disordered alloys we explicitly demonstrate that Bi atoms act as isovalent impurities when incorporated in dilute quantities in III-V (In)GaAs(P) materials, strongly perturbing the electronic structure of the valence band. We identify and quantify the causes and consequences of the unusual electronic properties of GaBixAs1−x and related alloys, and our analysis is reinforced throughout by a series of detailed comparisons to the results of experimental measurements. Our k•p models of the band structure of GaBixAs1−x and related alloys, which we derive directly from detailed atomistic calculations, are ideally suited to the study of dilute bismide-based devices. We focus in the latter part of the thesis on calculations of the electronic and optical properties of dilute bismide quantum well lasers. In addition to developing an understanding of the effects of Bi incorporation on the operational characteristics of semiconductor lasers, we also present calculations which have been used explicitly in designing and optimising the first generation of GaBixAs1−x-based devices.

Reformulating time-dependent density functional theory with non-orthogonal localized molecular orbitals.

Time-dependent density functional theory (TDDFT) has broad application in the study of electronic response, excitation and transport. To extend such application to large and complex systems, we develop a reformulation of TDDFT equations in terms of non-orthogonal localized molecular orbitals (NOLMOs). NOLMO is the most localized representation of electronic degrees of freedom and has been used in ground state calculations. In atomic orbital (AO) representation, the sparsity of NOLMO is transferred to the coefficient matrix of molecular orbitals (MOs). Its novel use in TDDFT here leads to a very simple form of time propagation equations which can be solved with linear-scaling effort. We have tested the method for several long-chain saturated and conjugated molecular systems within the self-consistent charge density-functional tight-binding method (SCC-DFTB) and demonstrated its accuracy. This opens up pathways for TDDFT applications to large bio- and nano-systems.

A stabilization mechanism of zirconia based on oxygen vacancies only

The microscopic mechanism leading to stabilization of cubic and tetragonal forms of zirconia (ZrO2) is analyzed by means of a self-consistent tight-binding model. Using this model, energies and structures of zirconia containing different vacancy concentrations are calculated, equivalent in concentration to the charge compensating vacancies associated with dissolved yttria (Y2O3) in the tetragonal and cubic phase fields (3.2 and 14.4% mol, respectively). The model is shown to predict the large relaxations around an oxygen vacancy, and the clustering of vacancies along the 111 directions, in good agreement with experiments and first principles calculations. The vacancies alone are shown to explain the stabilization of cubic zirconia, and the mechanism is analyzed. (C) 2002 Acta Materialia Inc. Published by Elsevier Science Ltd. All rights reserved.

Free energy and molecular dynamics calculations for the cubic-tetragonal phase transition in zirconia

The high-temperature cubic-tetragonal phase transition of pure stoichiometric zirconia is studied by molecular dynamics (MD) simulations and within the framework of the Landau theory of phase transformations. The interatomic forces are calculated using an empirical, self-consistent, orthogonal tight-binding model, which includes atomic polarizabilities up to the quadrupolar level. A first set of standard MD calculations shows that, on increasing temperature, one particular vibrational frequency softens. The temperature evolution of the free-energy surfaces around the phase transition is then studied with a second set of calculations. These combine the thermodynamic integration technique with constrained MD simulations. The results seem to support the thesis of a second-order phase transition but with unusual, very anharmonic behavior above the transition temperature.

Current-driven magnetic rearrangements in spin-polarized point contacts

A method for investigating the dynamics of atomic magnetic moments in current-carrying magnetic point contacts under bias is presented. This combines the nonequilibrium Green's function (NEGF) method for evaluating the current and the charge density with a description of the dynamics of the magnetization in terms of quasistatic thermally activated transitions between stationary configurations. This method is then implemented in a tight-binding (TB) model with parameters chosen to simulate the main features of the electronic structures of magnetic transition metals. We investigate the domain wall (DW) migration in magnetic monoatomic chains sandwiched between magnetic leads, and for realistic parameters find that collinear arrangement of the magnetic moments of the chain is always favorable. Several stationary magnetic configurations are identified, corresponding to a different number of Bloch walls in the chain and to a different current. The relative stability of these configurations depends on the geometrical details of the junction and on the bias; however, we predict transitions between different configurations with activation barriers of the order of a few tens of meV. Since different magnetic configurations are associated with different resistances, this suggests an intrinsic random telegraph noise at microwave frequencies in the I-V curves of magnetic atomic point contacts at room temperature. Finally, we investigate whether or not current-induced torques are conservative.

Inelastic current-voltage spectroscopy of atomic wires

A tight-binding model is developed to describe the electron-phonon coupling in atomic wires under an applied voltage and to model, their inelastic current-voltage spectroscopy. Particular longitudinal phonons are found to have greatly enhanced coupling to the electronic states of the system. This leads to a large drop in differential conductance at threshold energies associated with these phonons. It is found that with increasing tension these energies decrease, while the size of the conductance drops increases, in agreement with experiment.