arXiv subjects

John W. Wilkins

Publications and source records attributed to John W. Wilkins.

14 recordsLinked to original sources

arXiv2017

Ab initio based empirical potential applied to tungsten at high pressure

Density-functional theory forces, stresses and energies comprise a database from which the optimal parameters of a spline-based empirical potential combining Stillinger-Weber and modified embedded-atom forms are determined. Accuracy of the potential is demonstrated by predictions of ideal shear, stacking fault, vacancy migration, elastic constants and phonons all between 0 and 100 GPa. Consistency with existing models and experiments is demonstrated by application to screw dislocation core structure and deformation twinning in a tungsten nanorod. Lastly, the potential is used to study the high-pressure bcc to fcc phase transition.

cond-mat.mtrl-sci↗

arXiv2014

Comparison of polynomial approximations to speed up planewave-based quantum Monte Carlo calculations

The computational cost of quantum Monte Carlo (QMC) calculations of realistic periodic systems depends strongly on the method of storing and evaluating the many-particle wave function. Previous work [A. J. Williamson et al., Phys. Rev. Lett. 87, 246406 (2001); D. Alfè and M. J. Gillan, Phys. Rev. B 70, 161101 (2004)] has demonstrated the reduction of the O(N^3) cost of evaluating the Slater determinant with planewaves to O(N^2) using localized basis functions. We compare four polynomial approximations as basis functions -- interpolating Lagrange polynomials, interpolating piecewise-polynomial-form (pp-) splines, and basis-form (B-) splines (interpolating and smoothing). All these basis functions provide a similar speedup relative to the planewave basis. The pp-splines have eight times the memory requirement of the other methods. To test the accuracy of the basis functions, we apply them to the ground state structures of Si, Al, and MgO. The polynomial approximations differ in accuracy most strongly for MgO and smoothing B-splines most closely reproduce the planewave value for of the variational Monte Carlo energy. Using separate approximations for the Laplacian of the orbitals increases the accuracy sufficiently to justify the increased memory requirement, making smoothing B-splines, with separate approximation for the Laplacian, the preferred choice for approximating planewave-represented orbitals in QMC calculations.

physics.comp-ph↗

arXiv2012

Magnetic states and optical properties of single-layer carbon-doped hexagonal boron nitride

We show that carbon-doped hexagonal boron nitride (h-BN) has extraordinary properties with many possible applications. We demonstrate that the substitution-induced impurity states, associated with carbon atoms, and their interactions dictate the electronic structure and properties of C-doped h-BN. Furthermore, we show that stacking of localized impurity states in small C clusters embedded in h-BN forms a set of discrete energy levels in the wide gap of h-BN. The electronic structures of these C clusters have a plethora of applications in optics, magneto-optics, and opto-electronics.

cond-mat.mes-hall↗

arXiv2010

Band offsets of semiconductor heterostructures: a hybrid density functional study

We demonstrate the accuracy of the hybrid functional HSE06 for computing band offsets of semiconductor alloy heterostructures. The highlight of this study is the computation of conduction band offsets with a reliability that has eluded standard density functional theory. A high-quality special quasirandom structure models an infinite random pseudobinary alloy for constructing heterostructures along the (001) growth direction. Our excellent results for a variety of heterostructures establish HSE06's relevance to band engineering of high-performance electrical and optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2010

Accuracy of Quantum Monte Carlo Methods for Point Defects in Solids

Quantum Monte Carlo approaches such as the diffusion Monte Carlo (DMC) method are among the most accurate many-body methods for extended systems. Their scaling makes them well suited for defect calculations in solids. We review the various approximations needed for DMC calculations of solids and the results of previous DMC calculations for point defects in solids. Finally, we present estimates of how approximations affect the accuracy of calculations for self-interstitial formation energies in silicon and predict DMC values of 4.4(1), 5.1(1) and 4.7(1) eV for the X, T and H interstitial defects, respectively, in a 16(+1)-atom supercell.

cond-mat.mtrl-sci↗

arXiv2010

Accurate Ab-initio Predictions of III-V Direct-Indirect Band Gap Crossovers

We report the compositional dependence of the electronic band structure for a range of III-V alloys. Density functional theory with the PBE functional is insufficient to mimic the electronic gap energies at different symmetry points of the Brillouin zone. The HSE hybrid functional with screened exchange accurately reproduces the experimental band gaps and, more importantly, the alloy concentration of the direct-indirect gap crossovers for the III-V alloys studied here: AlGaAs, InAlAs, AlInP, InGaP, and GaAsP.

cond-mat.mtrl-sci↗

arXiv2010

Force-matched embedded-atom method potential for niobium

Large-scale simulations of plastic deformation and phase transformations in alloys require reliable classical interatomic potentials. We construct an embedded-atom method potential for niobium as the first step in alloy potential development. Optimization of the potential parameters to a well-converged set of density-functional theory (DFT) forces, energies, and stresses produces a reliable and transferable potential for molecular dynamics simulations. The potential accurately describes properties related to the fitting data, and also produces excellent results for quantities outside the fitting range. Structural and elastic properties, defect energetics, and thermal behavior compare well with DFT results and experimental data, e.g., DFT surface energies are reproduced with less than 4% error, generalized stacking-fault energies differ from DFT values by less than 15%, and the melting temperature is within 2% of the experimental value.

cond-mat.mtrl-sci↗

arXiv2005

Effects of morphology on phonons of nanoscopic silver grains

The morphology of nanoscopic Ag grains significantly affects the phonons. Atomistic simulations show that realistic nanograin models display complex vibrational properties. (1) Single-crystalline grains. Nearly-pure torsional and radial phonons appear at low frequencies. For low-energy, faceted models, the breathing mode and acoustic gap (lowest frequency) are about 10% lower than predicted by elasticity theory (ET) for a continuum sphere of the same volume. The sharp edges and the atomic lattice split the ET-acoustic-gap quintet into a doublet and triplet. The surface protrusions associated with nearly spherical, high-energy models produce a smaller acoustic gap and a higher vibrational density of states (DOS) at frequencies ν<2 THz. (2) Twined icosahedra. In contrast to the single-crystal case, the inherent strain produce a larger acoustic gap, while the core atoms yield a DOS tail extending beyond the highest frequency of single-crystalline grains. (3) Mark's decahedra, in contrast to (1) and (2), do not have a breathing mode; although twined and strained, do not exhibit a high-frequency tail in the DOS. (4) Irregular nanograins. Grain boundaries and surface disorder yield non-degenerate phonon frequencies, and significantly smaller acoustic gap. Only these nanograins exhibit a low-frequency ν^2 DOS in the interval 1-2 THz.

cond-mat.mtrl-sci↗

arXiv2005

Fast Diffusion Mechanism of Silicon Tri-interstitial Defects

We reveal the microscopic self-diffusion process of compact tri-interstitials in silicon using a combination of molecular dynamics and nudged elastic band methods. We find that the compact tri-interstitial moves by a collective displacement, involving both translation and rotation, of five atoms in a screw-like motion along $[111]$ directions. The elucidation of this pathway demonstrates the utility of combining tight-binding molecular dynamics with \textit{ab initio} density functional calculations to probe diffusion mechanisms. Using density functional theory to obtain diffusion barriers and the prefactor, we calculate a diffusion constant of $ 4 \cdot 10^{-5} \exp (- 0.49 {\rm eV} / k_{B} T) {\rm cm^2/s} $. Because of the low diffusion barrier, $I_{3}^{b}$ diffusion may be an important process under conditions such as ion implantation that creates excess interstitials, hence favoring formation of interstitial clusters.

cond-mat.mtrl-sci↗

arXiv2000

Electron-hole correlations in semiconductor quantum dots with tight-binding wave functions

The electron-hole states of semiconductor quantum dots are investigated within the framework of empirical tight-binding descriptions for Si, as an example of an indirect gap material, and InAs and CdSe as examples of typical III-V and II-VI direct-gap materials. The electron-hole Coulomb interaction is largely insensitive to both the real-space description of the atomic basis orbitals and different ways of optimizing the tight-binding parameters. Tight-binding parameters that are optimized to give the best effective masses significantly improve the energies of the excitonic states due to the better single-particle energies. However, the Coulomb interaction does not vary much between different parameterizations. In addition, the sensitivity of the Coulomb interaction to the choice of atomic or bitals decreases with increasing dot size. Quantitatively, tight-binding treatments of correlation effects are reliable for dots with radii larger than 15--20 angstrom. The calculated excitonic gaps are in good agreement with recent photoluminescence data for Si and CdSe but agree less well for InAs. Further, the effective range of the electron-hole exchange interaction is investigated in detail. In quantum dots of the direct-gap materials InAs and CdSe, the exchange interaction can be long-ranged, extending over the whole dot when there is no local (onsite) orthogonality between the electron and hole wave functions. By contrast, for Si quantum dots the extra phase factor due to the indirect gap effectively limits the range to about 15 angstrom, independent of the dot size.

cond-mat↗

arXiv1996

Extended Si defects

We perform total energy calculations based on the tight-binding Hamiltonian scheme (i) to study the structural properties and energetics of the extended {311} defects depending upon their dimensions and interstitial concentrations and (ii) to find possible mechanisms of interstitial capture by and release from the {311} defects. The generalized orbital-based linear-scaling method implemented on Cray-T3D is used for supercell calculations of large scale systems containing more than 1000 Si atoms.

cond-mat.mtrl-sci↗

arXiv1996

Optical conductivity associated with solitons in the Peierls state as modified by zero-point-motion disorder

We extend previous work to consider the effect of the soliton on the density of states and conductivity of quasi-one-dimensional Peierls systems with quantum lattice fluctuations, modeled by a random static disorder. Two features have been verified over an order of magnitude variation in the disorder. (1) The soliton density of states and the leading edges of both the soliton-to-band and the band-to-band conductivities have universal scaling forms. (2) The soliton-to-band conductivity has the remarkable feature that the leading edge is accurately predicted by the joint density of states while the trailing edge tracks the rigid-lattice conductivity. Or, in other words, disorder dominates the leading edge, while matrix element effects are predominant for the trailing edge.

cond-mat↗

arXiv1993

Universal subgap optical conductivity in quasi-one-dimensional Peierls systems

Quasi-one-dimensional Peierls systems with quantum and thermal lattice fluctuations can be modeled by a Dirac-type equation with a Gaussian-correlated off-diagonal disorder. A powerful new method gives the exact disorder-averaged Green function used to compute the optical conductivity. The strong subgap tail of the conductivity has a universal scaling form. The frequency and temperature dependence of the calculated spectrum agrees with experiments on KCP(Br) and trans-polyacetylene.

cond-mat↗

arXiv1992

Zero Frequency Current Noise for the Double Tunnel Junction Coulomb Blockade

We compute the zero frequency current noise numerically and in several limits analytically for the coulomb blockade problem consisting of two tunnel junctions connected in series. At low temperatures over a wide range of voltages, capacitances, and resistances it is shown that the noise measures the variance in the number of electrons in the region between the two tunnel junctions. The average current, on the other hand, only measures the mean number of electrons. Thus, the noise provides additional information about transport in these devices which is not available from measuring the current alone.

cond-mat↗