Silica glass structure generation for ab initio calculations using small samples of amorphous silica

Multiple small samples of amorphous silica have been generated and optimized using classical dynamics and the van Beest-Kramer-van Santen sBKSd empirical potential function. The samples were subsequently optimized and annealed using density functional theory sDFTd with both the local density and the generalized gradient approximations. A thorough analysis of the local and medium-range structure of the optimized samples obtained from the different methods was carried out. The structural characteristics obtained for the average of small systems each containing ca. 100 ions are compared for each of the different methods, and to the BKS simulation of a larger system. The differences found between the DFT and BKS simulations and the effects of volume relaxation on the structures are discussed. Fixed-volume samples are compared to neutron scattering data, with good agreement to 5 A, the length limit of the sample sizes used here. It is shown that by creating multiple small samples, it is possible to achieve a good statistical sampling of structural features consistent with larger simulated glass systems. This study also shows that multiple small samples are necessary to capture the structural distribution of silica glass, and therefore to study more complex processes in glass, such as reactions.

[1]  D. Vanderbilt,et al.  Soft self-consistent pseudopotentials in a generalized eigenvalue formalism. , 1990, Physical review. B, Condensed matter.

[2]  D. Hamann.  Diffusion of Atomic Oxygen in SiO 2 , 1998 .

[3]  N. Mermin.  Thermal Properties of the Inhomogeneous Electron Gas , 1965 .

[4]  W Smith,et al.  DL_POLY_2.0: a general-purpose parallel molecular dynamics simulation package. , 1996, Journal of molecular graphics.

[5]  A. Stoneham,et al.  Role of disorder in incorporation energies of oxygen atoms in amorphous silica , 2001 .

[6]  Martins,et al.  Efficient pseudopotentials for plane-wave calculations. , 1991, Physical review. B, Condensed matter.

[7]  P. Wolynes,et al.  Intrinsic quantum excitations of low temperature glasses. , 2001, Physical review letters.

[8]  G. Barkema,et al.  Traveling through potential energy landscapes of disordered materials: The activation-relaxation technique , 1997, cond-mat/9710023.

[9]  M. Benoit,et al.  Signature of small rings in the Raman spectra of normal and compressed amorphous silica: A combined classical and ab initio study , 2003, cond-mat/0308164.

[10]  R. Car,et al.  Dynamic structure factor of vitreous silica from first principles: Comparison to neutron-inelastic-scattering experiments , 1998 .

[11]  János G. Ángyán,et al.  Polymorphism in silica studied in the local density and generalized-gradient approximations , 1999 .

[12]  A. Edwards,et al.  Calibration of embedded-cluster method for defect studies in amorphous silica , 2004 .

[13]  H. C. Andersen,et al.  Molecular dynamics simulation of silica liquid and glass , 1992 .

[14]  Alfredo Pasquarello,et al.  Identification of Raman defect lines as signatures of ring structures in vitreous silica , 1998 .

[15]  Xianglong Yuan,et al.  Efficient algorithm for primitive ring statistics in topological networks , 2002 .

[16]  Lee,et al.  Implementation of ultrasoft pseudopotentials in ab initio molecular dynamics. , 1991, Physical review. B, Condensed matter.

[17]  G. Kresse,et al.  Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set , 1996 .

[18]  C. Angell,et al.  Molecular dynamics studies of the vitreous state: Simple ionic systems and silica , 1976 .

[19]  W. Kohn,et al.  Self-Consistent Equations Including Exchange and Correlation Effects , 1965 .

[20]  Car,et al.  Model of vitreous SiO2 generated by an ab initio molecular-dynamics quench from the melt. , 1995, Physical review. B, Condensed matter.

[21]  Binder,et al.  Finite size effects in simulations of glass dynamics. , 1996, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[22]  A. Zunger,et al.  Self-interaction correction to density-functional approximations for many-electron systems , 1981 .

[23]  A. Stoneham,et al.  Atomistic modelling of radiation effects: Towards dynamics of exciton relaxation , 2000 .

[24]  A. Cormack,et al.  Si–O–Si bond angle and torsion angle distribution in vitreous silica and sodium silicate glasses , 2003 .

[25]  L. Hobbs,et al.  Molecular dynamics refinement of topologically generated reconstructions of simulated irradiation cascades in silica networks , 2001 .

[26]  D. Hamann.  Energies of strained silica rings , 1997 .

[27]  A. Cormack,et al.  Local structures of MD-modeled vitreous silica and sodium silicate glasses , 2001 .

[28]  Hamann.  Generalized gradient theory for silica phase transitions. , 1996, Physical review letters.

[29]  Binder,et al.  Cooling-rate effects in amorphous silica: A computer-simulation study. , 1996, Physical review. B, Condensed matter.

[30]  Hafner,et al.  Ab initio molecular-dynamics simulation of the liquid-metal-amorphous-semiconductor transition in germanium. , 1994, Physical review. B, Condensed matter.

[31]  Kramer,et al.  Force fields for silicas and aluminophosphates based on ab initio calculations. , 1990, Physical review letters.

[32]  A. E. Geissberger,et al.  Raman studies of vitreous Si O 2 versus fictive temperature , 1983 .

[33]  F. L. Galeener,et al.  Planar rings in vitreous silica , 1982 .

[34]  L. Corrales,et al.  Molecular Dynamics Simulation of La2O3-Na2O-SiO2 Glasses: I. The Structural Role of La3+ Cations , 2002 .

[35]  Car,et al.  Structural and electronic properties of liquid and amorphous SiO2: An ab initio molecular dynamics study. , 1995, Physical review letters.

[36]  G. Kresse,et al.  Ab initio molecular dynamics for liquid metals. , 1993 .

[37]  A. Cormack,et al.  Molecular dynamics simulations of structural changes in mixed alkali (Li–K) silicate glasses , 1999 .

[38]  H. Jónsson,et al.  Self-trapped excitons in quartz , 2000 .

[39]  Thomas R Huser,et al.  Modification of the fused silica glass network associated with waveguide fabrication using femtosecond laser pulses , 2003 .

[40]  A. Wright.  Neutron and X-ray amorphography , 1988 .

[41]  Kresse,et al.  Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. , 1996, Physical review. B, Condensed matter.

[42]  James B. Adams,et al.  Application of design of experiments methodology to optimization of classical molecular dynamics generation of amorphous SiO2 structure , 2004 .

[43]  S. Nosé.  A unified formulation of the constant temperature molecular dynamics methods , 1984 .

[44]  W. Kob,et al.  NUMERICAL STUDY OF THE ELECTRONIC STRUCTURE OF AMORPHOUS SILICA , 1997 .

[45]  R. Car,et al.  DYNAMICAL CHARGE TENSORS AND INFRARED SPECTRUM OF AMORPHOUS SIO2 , 1997 .

[46]  P. P. Ewald.  Die Berechnung optischer und elektrostatischer Gitterpotentiale , 1921 .

[47]  A. Cormack,et al.  Molecular Dynamics Simulations of Silicate Glasses and Melts , 2001 .

[48]  Magali Benoit,et al.  Model of silica glass from combined classical and ab initio molecular-dynamics simulations , 2000 .

[49]  H. Berendsen,et al.  Molecular dynamics with coupling to an external bath , 1984 .

[50]  Structural properties of molten silicates from ab initio molecular-dynamics simulations: Comparison between (formula presented) and (formula presented) , 2001, cond-mat/0109267.

[51]  C. Brinker,et al.  Relationship between strained silicon-oxygen bonds and radiation induced paramagnetic point defects in silicon dioxide , 1991 .

[52]  A. Wright.  The comparison of molecular dynamics simulations with diffraction experiments , 1993 .

[53]  N. T. Huff,et al.  Factors affecting molecular dynamics simulated vitreous silica structures , 1999 .

[54]  S T Pantelides,et al.  Reactions and diffusion of water and oxygen molecules in amorphous SiO2. , 2002, Physical review letters.

[55]  Berend Smit,et al.  Understanding Molecular Simulation , 2001 .

[56]  Jackson,et al.  Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation. , 1992, Physical review. B, Condensed matter.