First-principles study of transition metal impurities in Si

By using ab initio electronic structure calculations within density functional theory, we study the structural, electronic, and magnetic properties of Si doped with a transition metal impurity. We consider the transition metals of the 3d series V, Cr, Mn, Fe, Co, and Ni. To get insight into the level filling mechanism and the magnetization saturation, we first investigate the transition metal-Si alloys in the zinc-blende structure. Next, we investigate the doping of bulk Si with a transition metal atom, in which it occupies the substitutional site, the interstitial site with tetrahedral symmetry, and the interstitial site with hexagonal symmetry. It is found that all of these transition metal impurities prefer an interstitial position in Si. Furthermore, we show that it is possible to interpret the electronic and magnetic properties by using a simple level filling picture and a comparison is made to Ge doped with the same transition metal atoms. In order to get insight into the effect of a strained environment, we calculate the formation energy as a function of an applied homogeneous pressure and we show that an applied pressure can stabilize the substitutional position of transition metal impurities in Si. Finally, the energies of the ferromagnetic states are compared to those of the antiferromagnetic states. It is shown that the interstitial site of the Mn dopant helps us to stabilize the nearest neighbor substitutional site to realize the ferromagnetic state. For doping of Si with Cr, a ferrimagnetic behavior is predicted.

A density-functional study of Al-doped Ti clusters: TinAl (n=1-13)

Equilibrium geometries, stabilities, and electronic properties of TinAl (n=1-13) clusters have been studied by using density-functional theory with local spin density approximation and generalized gradient approximation. The ground-state structures of TinAl clusters have been obtained. The resulting geometries show that the aluminum atom remains on the surface of clusters for n<9, but is slowly getting trapped beyond n=9, meanwhile, the Al atom exhibits a valent transition from monovalent to trivalent. The geometric effects and electronic effects clearly demonstrate the Ti4Al cluster to be endowed with special stability. The studies on the bonds indicate the change from ionic to metalliclike. (C) 2004 American Institute of Physics.

Effective-mass theory for hierarchical self-assembly of GaAs/AlxGa1-xAs quantum dots

The electronic structures in the hierarchical self-assembly of GaAs/AlxGa1-xAs quantum dots are investigated theoretically in the framework of effective-mass envelope function theory. The electron and hole energy levels and optical transition energies are calculated. In our calculation, the effect of finite offset, valence-band mixing, the effects due to the different effective masses of electrons and holes in different regions, and the real quantum dot structures are all taken into account. The results show that (1) electronic energy levels decrease monotonically, and the energy difference between the energy levels increases as the GaAs quantum dot (QD) height increases; (2) strong state mixing is found between the different energy levels as the GaAs QD width changes; (3) the hole energy levels decrease more quickly than those of the electrons as the GaAs QD size increases; (4) in excited states, the hole energy levels are closer to each other than the electron ones; (5) the first heavy- and light-hole transition energies are very close. Our theoretical results agree well with the available experimental data. Our calculated results are useful for the application of the hierarchical self-assembly of GaAs/AlxGa1-xAs quantum dots to photoelectric devices.

Effective-mass theory for coupled quantum dots grown on (11N)-oriented substrates

The electronic structures of coupled quantum dots grown on (11N)-oriented substrates are studied in the framework of effective-mass envelope-function theory. The results show that the all-hole subbands have the smallest widths and the optical properties are best for the (113), (114), and (115) growth directions. Our theoretical results agree with the available experimental data. Our calculated results are useful for the application of coupled quantum dots in photoelectric devices.

InAs/GaAs single-electron quantum dot qubit

The time evolution of the quantum mechanical state of an electron is calculated in the framework of the effective-mass envelope function theory for an InAs/GaAs quantum dot. The results indicate that the superposition state electron density oscillates in the quantum dot, with a period on the order of femtoseconds. The interaction energy E-ij between two electrons located in different quantum dots is calculated for one electron in the ith pure quantum state and another in the jth pure quantum state. We find that E-11]E-12]E-22, and E-ij decreases as the distance between the two quantum dots increases. We present a parameter-phase diagram which defines the parameter region for the use of an InAs/GaAs quantum dot as a two-level quantum system in quantum computation. A static electric field is found to efficiently prolong the decoherence time. Our results should be useful for designing the solid-state implementation of quantum computing. (C) 2001 American Institute of Physics.

A density-functional study of small titanium clusters

The atomic structures and electronic properties of small Ti-N (N=2-10) clusters have been studied by using the density-functional theory with a local spin density approximation. We find that the inner-shells (3s3p) of the titanium atom plays an important role in the formation of the small clusters. We have obtained the ground state of titanium clusters, Ti-7 is found to be a magic cluster, which is in good agreement with the experimental results. Starting with Ti-8 cluster some features of the electronic structure of the titanium bulk have been developed. The ionization potentials and magnetic moments for these small titanium clusters are also presented. (C) 2000 American Institute of Physics. [S0021- 9606(00)30544-X].

Linear and nonlinear intersubband optical properties in a step quantum well with an applied electric field

Within the framework of the effective-mass envelope-function theory, the field-dependent intersubband optical properties of a Al0.4Ga0.6As/Al0.2Ga0.8As/GaAs step quantum well are investigated theoretically based on the periodic boundary condition. A very large Stark shift occurs when the lowest subband electron remains confined to the small well while the higher subband electron confined to the big well. The optical nonlinearity in a step well due to resonant intersubband transition (ISBT) is analyzed using a density-matrix approach. The second-harmonic generation coefficient chi(2 omega)((2)) and nonlinear optical rectification chi(0)((2)) have also been investigated theoretically. The results show that the ISBT in a step well can generate very large second order optical nonlinearities, chi(0)((2)) and chi(2 omega)((2)) can be tuned by the electric field over a wide range.

Electronic, structural, and optical properties of crystalline yttria

The electronic structure of crystalline Y2O3 is investigated by first-principles calculations within the local-density approximation (LDA) of the density-functional theory. Results are presented for the band structure, the total density of states (DOS), the atom-and orbital-resolved partial DOS. effective charges, bond order, and charge-density distributions. Partial covalent character in the Y-O bonding is shown, and the nonequivalency of the two Y sites is demonstrated. The calculated electronic structure is compared with a variety of available experimental data. The total energy of the crystal is calculated as a function of crystal volume. A bulk modulus B of 183 Gpa and a pressure coefficient B' of 4.01 are obtained, which are in good agreement with compression data. An LDA band gap of 4.54 eV at Gamma is obtained which increases with pressure at a rate of dE(g)/dP = 0.012 eV/Gpa at the equilibrium volume. Also investigated are the optical properties of Y2O3 up to a photon energy of 20 eV. The calculated complex dielectric function and electron-energy-loss function are in good agreement with experimental data. A static dielectric constant of epsilon(O)= 3.20 is obtained. It is also found that the bottom of the conduction band consists of a single band, and direct optical transition at Gamma between the top of the valence band and the bottom of the conduction band may be symmetry forbidden.

1ST-PRINCIPLES CALCULATIONS FOR QUASI-PARTICLE ENERGIES OF GAP AND GAAS

We have applied the Green-function method in the GW approximation to calculate quasiparticle energies for the semiconductors GaP and GaAs. Good agreement between the calculated excitation energies and the experimental results was achieved. We obtained calculated direct band gaps of GaP and GaAs of 2.93 and 1.42 eV, respectively, in comparison with the experimental values of 2.90 and 1.52 eV, respectively. An ab initio pseudopotential method has been used to generate basis wave functions and charge densities for calculating the dielectric matrix elements and self-enegies. To evaluate the dynamical effects of the screened interaction, the generalized-plasma-pole model has been utilized to extend the dielectric matrix elements from static results to finite frequencies. We presen the calculated quasiparticle energies at various high-symmetry points of the Brillouin zone and compare them with the experimental results and other calculations.

1ST PRINCIPLE CALCULATIONS OF QUASI-PARTICLE ENERGIES FOR BAND STRUCTURES OF SEMICONDUCTORS

We successfully applied the Green function theory in GW approximation to calculate the quasiparticle energies for semiconductors Si and GaAs. Ab initio pseudopotential method was adopted to generate basis wavefunctions and charge densities for calculating dielectric matrix elements and electron self-energies. To evaluate dynamical effects of screened interaction, GPP model was utilized to extend dieletric matrix elements from static results to finite frequencies. We give a full account of the theoretical background and the technical details for the first principle pseudopotential calculations of quasiparticle energies in semiconductors and insulators. Careful analyses are given for the effective and accurate evaluations of dielectric matrix elements and quasiparticle self-energies by using the symmetry properties of basis wavefunctions and eigenenergies. Good agreements between the calculated excitation energies and fundamental energy gaps and the experimental band structures were achieved.

Effective-mass theory for InAs/GaAs strained superlattices

By using the recently developed exact effective-mass envelope-function theory, the electronic structures of InAs/GaAs strained superlattices grown on GaAs (100) oriented substrates are studied. The electron and hole subband structures, distribution of electrons and holes along the growth direction, optical transition matrix elements, exciton states, and absorption spectra are calculated. In our calculations, the effects due to the different effective masses of electrons and holes in different materials and the strain are included. Our theoretical results are in agreement with the available experimental data.

Effective-mass theory for InAs/GaAs strained coupled quantum dots

In the framework of effective-mass envelope-function theory, the optical transitions of InAs/GaAs strained coupled quantum dots grown on GaAs (100) oriented substrates are studied. At the Gamma point, the electron and hole energy levels, the distribution of electron and hole wave functions along the growth and parallel directions, the optical transition-matrix elements, the exciton states, and absorption spectra are calculated. In calculations, the effects due to the different effective masses of electrons and holes in different materials are included. Our theoretical results are in good agreement with the available experimental data.

First principles based predictions of the toughness of a metal/oxide interface

We describe a first-principles-based strategy to predict the macroscopic toughness of a gamma-Ni(Al)/alpha-Al2O3 interface. Density functional theory calculations are used to ascertain energy changes upon displacing the two materials adjacent to the interface, with relaxation conducted over all atoms located within adjoining rows. Traction/displacernent curves are obtained from derivatives of the energy. Calculations are performed in mode I (opening), mode II (shear) and at a phase angle of 45 degrees. The shear calculations are conducted for displacements along < 110 > and < 112 > of the Ni lattice. A generalized interface potential function is used to characterize the results. Initial fitting to both the shear and normal stress results is required to calibrate the unknowns. Thereafter, consistency is established by using the potential to predict other traction quantities. The potential is incorporated as a traction/displacement function within a cohesive zone model and used to predict the steady-state toughness of the interface. For this purpose, the plasticity of the Ni alloy must be known, including the plasticity length scale. Measurements obtained for a gamma-Ni superalloy are used and the toughness predicted over the full range of mode mixity. Additional results for a range of alloys are used to demonstrate the influences of yield strength and length scale.

First principles based predictions of the toughness of a metal/oxide interface

We describe a first-principles-based strategy to predict the macroscopic toughness of a gamma-Ni(Al)/alpha-Al2O3 interface. Density functional theory calculations are used to ascertain energy changes upon displacing the two materials adjacent to the interface, with relaxation conducted over all atoms located within adjoining rows. Traction/displacernent curves are obtained from derivatives of the energy. Calculations are performed in mode I (opening), mode II (shear) and at a phase angle of 45 degrees. The shear calculations are conducted for displacements along < 110 > and < 112 > of the Ni lattice. A generalized interface potential function is used to characterize the results. Initial fitting to both the shear and normal stress results is required to calibrate the unknowns. Thereafter, consistency is established by using the potential to predict other traction quantities. The potential is incorporated as a traction/displacement function within a cohesive zone model and used to predict the steady-state toughness of the interface. For this purpose, the plasticity of the Ni alloy must be known, including the plasticity length scale. Measurements obtained for a gamma-Ni superalloy are used and the toughness predicted over the full range of mode mixity. Additional results for a range of alloys are used to demonstrate the influences of yield strength and length scale.

TIME-DEPENDENT DENSITY FUNCTIONAL STUDY OF MULTIELECTRON TRANSFER IN Cq+-Na-4 COLLISIONS

The process of multielectron transfer from a Na-4 cluster induced by highly charged C6+, C4+, C2+ and C+ ions is studied using the method of time-dependent density functional theory within the local density approximation combined with the use of pseudopotential. The evolution of dipole moment changes and emitted electrons in Na-4 isobtained and the time-dependent probabilities with various charges are deduced. It is shown that the Na-4 cluster is strongly ionized by C6+ and that the number of emitted electrons per atom of Na-4 is larger than that of Na-2 under the same condition. One can find that the detailed information of the emitted electrons from Na-4 is different from the same from Na-2, which is possibly related to the difference in structure between the two clusters.