ab inito local vibrational modes of light impurities in silicon

We have developed a formulation of density functional perturbation theory for the calculation of vibrational frequencies in molecules and solids, which uses numerical atomic orbitals as a basis set for the electronic states. The (harmonic) dynamical matrix is extracted directly from the first order change in the density matrix with respect to infinitesimal atomic displacements from the equilibrium configuration. We have applied this method to study the vibrational properties of a number of hydrogen-related complexes and light impurities in silicon. The diagonalization of the dynamical matrix provides the vibrational modes and frequencies, including the local vibrational modes (LVMs) associated with the defects. In addition to tests on simple molecules, results for interstitial hydrogen, hydrogen dimers, vacancy-hydrogen and self-interstitial-hydrogen complexes, the boron-hydrogen pair, substitutional C, and several O-related defects in c-Si are presented. The average error relative to experiment for the aprox.60 predicted LVMs is about 2% with most highly harmonic modes being extremely close and the more anharmonic ones within 5-6% of the measured values.Comment: 18 pages, 1 figur

Hydrogenation Methods and Passivation Mechanisms for c-Si Photovoltaics: Final Technical Report, 2 January 2002 - 15 January 2008

Joint experimental and theortetical research program to improve processes used to eliminate or passivate lifetime-reducing defects in the Si bulk

Heat capacity of α\alpha-GaN: Isotope Effects

Until recently, the heat capacity of GaN had only been measured for polycrystalline powder samples. Semiempirical as well as \textit{first-principles} calculations have appeared within the past few years. We present in this article measurements of the heat capacity of hexagonal single crystals of GaN in the 20-1400K temperature range. We find that our data deviate significantly from the literature values for polycrystalline materials. The dependence of the heat capacity on the isotopic mass has also been investigated recently for monatomic crystals such as diamond, silicon, and germanium. Multi-atomic crystals are expected to exhibit a different dependence of these heat capacities on the masses of each of the isotopes present. These effects have not been investigated in the past. We also present \textit{first-principles} calculations of the dependence of the heat capacities of GaN, as a canonical binary material, on each of the Ga and N masses. We show that they are indeed different, as expected from the fact that the Ga mass affects mainly the acoustic, that of N the optic phonons. It is hoped that these calculations will encourage experimental measurements of the dependence of the heat capacity on isotopic masses in binary and more complex semiconductors.Comment: 12 pages, 5 Figures, submitted to PR

Stable fourfold configurations for small vacancy clusters in silicon from ab initio calculations

Using density-functional-theory calculations, we have identified new stable configurations for tri-, tetra-, and penta-vacancies in silicon. These new configurations consist of combinations of a ring-hexavacancy with three, two, or one interstitial atoms, respectively, such that all atoms remain fourfold. As a result, their formation energies are lower by 0.6, 1.0, and 0.6 eV, respectively, than the ``part of a hexagonal ring'' configurations, believed up to now to be the lowest-energy states

Thermal conductivity of Si nanostructures containing defects: Methodology, isotope effects, and phonon trapping

A first-principles method to calculate the thermal conductivity in nanostructures that may contain defects or impurities is described in detail. The method mimics the so-called "laser-flash" technique to measure thermal conductivities. It starts with first-principles density-functional theory and involves the preparation of various regions of a supercell at slightly different temperatures. The temperature fluctuations are minimized without using a thermostat and, after averaging over random initial conditions, temperature changes as small as 5 K can be monitored (from 120 to 125 K). The changes to the phonon density of states and the specific heat induced by several atomic percent of impurities are discussed. The thermal conductivity of Si supercells is calculated as a function of the temperature and of the impurity content. For most impurities, the drop in thermal conductivity is unremarkable. However, there exist narrow ranges of impurity parameters (mass, bond strength, etc.) for which substantial drops in the thermal conductivity are predicted. These drops are isotope dependent and appear to be related to the vibrational lifetime of specific impurity-related modes

Reversal of the Charge Transfer between Host and Dopant Atoms in Semiconductor Nanocrystals

We present ab initio density functional calculations that show P (Al) dopant atoms in small hydrogen-terminated Si crystals to be negatively (positively) charged. These signs of the dopant charges are reversed relative to the same dopants in bulk Si. We predict this novel reversal of the dopant charge (and electronic character of the doping) to occur at crystal sizes of order 100 Si atoms. We explain it as a result of competition between fundamental principles governing charge transfer in bulk semiconductors and molecules and predict it to occur in nanocrystals of most semiconductors.Comment: 4 pages, 4 figures (3 in color), 2 table

Nickel: A very fast diffuser in silicon

Nickel is increasingly used in both IC and photovoltaic device fabrication, yet it has the potential to create highly recombination-active precipitates in silicon. For nearly three decades, the accepted nickel diffusivity in silicon has been DNi(T)=2.3×10exp−3 exp(−0.47 eV/kBT) cm2/s, a surprisingly low value given reports of rapid nickel diffusion in industrial applications. In this paper, we employ modern experimental methods to measure the higher nickel diffusivity DNi(T)=(1.69±0.74)×10exp−4 exp(−0.15±0.04 eV/kBT)  cm2/s. The measured activation energy is close to that predicted by first-principles theory using the nudged-elastic-band method. Our measured diffusivity of nickel is higher than previously published values at temperatures below 1150 °C, and orders of magnitude higher when extrapolated to room temperature.Peer reviewe

Suppression of decoherence via strong intra-environmental coupling

We examine the effects of intra-environmental coupling on decoherence by constructing a low temperature spin--spin-bath model of an atomic impurity in a Debye crystal. The impurity interacts with phonons of the crystal through anti-ferromagnetic spin-spin interactions. The reduced density matrix of the central spin representing the impurity is calculated by dynamically integrating the full Schroedinger equation for the spin--spin-bath model for different thermally weighted eigenstates of the spin-bath. Exact numerical results show that increasing the intra-environmental coupling results in suppression of decoherence. This effect could play an important role in the construction of solid state quantum devices such as quantum computers.Comment: 4 pages, 3 figures, Revtex fil