Springer Nature is making SARS-CoV-2 and COVID-19 research free. View research | View latest news | Sign up for updates

Quantum mechanical potential surfaces and calculations on minerals and molecular clusters

I. STO-3G and 6-31G* results

  • 85 Accesses

  • 66 Citations

Abstract

Recently, ab-initio quantum mechanical potential surfaces calculated for silicate hydroxyacid molecules were used to extract covalent potentials for use in mineral physics calculations (Lasaga and Gibbs 1987). The calculations showed that these potentials are capable of generating the structure and physical properties of silicate minerals. In this paper we explore in more detail the suitability of various covalent potentials in mimicking the topography of the ab-initio potential surfaces. We also extend the use of such quantum-derived potentials in generating the structures of hydroxyacid dimers, trimers, and pentamers of silicate tetrahedra and in studying the structure and the dynamical properties of minerals and glasses.

This is a preview of subscription content, log in to check access.

References

  1. Basile LJ, Ferraro JR, LaBonville P, Wall MC, (1973) Force fields for tetrahedral molecules. Coord Chem Rev 11:21–69

  2. Born M, Huang K (1959) Dynamical theory of crystal lattices. Oxford: The Clarendon Press, p 327

  3. Brawer S (1983) Ab initio calculation of the vibration spectra of BeF2 glass simulated by molecular dynamics. J Chem Phys 79:4539–4544

  4. Busing WR (1981) WMIN, A computer program to model molecules and crystals in terms of potential energy functions. Oak Ridge Natl Lab Pub 5747

  5. Catlow CRA, Norgett MJ (1973) Shell model calculations of the energies of formation of point defects in alkaline earth fluorides. J Phys C 6:1325–1339

  6. Catlow CRA (1980) Computer modelling of ionic crystals. J Phys 41:C6–53

  7. Catlow CRA, Thomas JM, Parker SC, Jefferson DA (1982) Simulating silicate structures and the structural chemistry of pyroxenoids. Nature 295:658–662

  8. Chandler D (1974) Equilibrium structure and molecular motion in liquids. Acc Chem Res 7:246–251

  9. Cohen AJ, Gordon RG (1976) Modified electron-gas study of the stability, elastic properties and high-pressure bahavior of MgO and CaO crystals. Phys Rev Sect B 14:4503–4605

  10. Dean P (1972) Reviews of modern physics 44:127

  11. Garofalini SH, Melman H (1986) Application of molecular dynamics simulations to sol-gel processing, in belter ceramics through chemislry II, Vol 73, Materials Research Sociely, Symposia Proceedings, Brinker CJ, Clark VE, Ulrich DR (eds), pp 497–505

  12. Geisinger KL, Gibbs GV, Navrotsky A (1985) A molecular orbital study of bond length and angle variations in framework structures. Phys Chem Minerals 11:266–283

  13. Gibbs GV, Meagher EP, Newton MD, Swanson DI (1981) A comparison of experimental and theoretical bond lengths and angle variations for minerals, inorganic solids, and molecules, structure and bonding in crystals. Academic Press, Inc New York. Vol 1, pp 195–225

  14. Gibbs GV (1982) Molecules as models for bonding in silicates. Am Mineral 67:421–450

  15. Gibbs GV, D'Arco P, Boisen MB Jr (1987) Molecular mimicry of bond length and angle variations in germanate and thiogermanate crystals: A comparison with variations calculated for C-, Si- and SN-containing oxide and sulfide molecules. J Phys Chem 91:5347–5354

  16. Gordon RG, Kim YS (1972) Theory for the forces between closedshell atoms and molecules. J Chem Phys 56:3122–3133

  17. Jackson MD (1986) Theoretical investigations of chemical bonding in minerals. PhD Thesis, Harvard University

  18. Lasaga AC, Aerni R, Karplus M (1980) Photodynamics of polyenes I: The effect of electron correlation on potential surfaces. J Chem Phys 73:5230–5243

  19. Lasaga AC, Gibbs GV (1987) Quantum mechanical potentials and the structure of minerals. Phys Chem Minerals 14:107–117

  20. Longuet-Higgins HC, Widom B (1964) A rigid sphere model for the melting of argon. Mol Phys 8:549–556

  21. McMillan P (1984) A Raman spectroscopic study of glasses in the system CaO-MgO-SiO2. Am Mineral 69:645–659

  22. McMillan P (1984) Structural studies of silicate glasses and melts — applications and limitations of Raman spectroscopy. Am Mineral 69:622–644

  23. Mitra SK, Amini M, Fincham D, Hockney RW (1981) Molecular dynamics simulation of silicon dioxide glass. Philos Mag B 43:365–372

  24. Miyamoto M, Takeda H (1984) An attempt to simulate high pressure structures of Mg-silicates by an energy minimization method. Am Mineral 69:711–718

  25. Newton MD, Gibbs GV (1980) ab-initio calculated geometries and charge distributions for H4SiO4 and H6Si2O7 compared with experimenlal values for silicates and siloxanes. Phys Chem Minerals 6:221–246

  26. O'Keeffe M, Newton MD, Gibbs GV (1980) ab-initio calculation of interatomic force constants in H6Si2O7 and the bulk modulus of a quartz and a cristobalite. Phys Chem Minerals 6:305–312

  27. Parker SC (1983) Prediction of mineral crystal structures. Solid Slate Ionics 8:179–186

  28. Pauling L (1980) The nature of silicon-oxygen bonds. Am Mineral 65:321–323

  29. Piriou B, McMillan P (1983) The high-frequency vibrational spectra of vitreous and crystalline orthosilicates. Am Mineral 68:426–443

  30. Post J, Burnham CW (1986) Ionic models of mineral structures and energies in the electron gas approximation: TiO2 polymorphs, quartz, forsterite, diopside. Am Mineral 71:142–150

  31. Price GD, Parker SC (1984) Computer simulations of the structural and physical properties of the olivine and spinel polymorphs of Mg2SiO4. Phys Chem Minerals 10:209–216

  32. Stewart RF, Whitehead MA, Donnay G (1980) The ionicity of the Si-O bond in low-quartz. Am Mineral 65:324–326

  33. Tossell JA, Gibbs GV (1977) Molecular orbital studies of geometries and spectra of minerals and inorganic compounds. Phys Chem Minerals 2:21–57

  34. White WB (1975) Structural interpretation of lunar and terrestial minerals by Raman spectroscopy. Chapt 13 in: Infrared and Raman spectroscopy of lunar and terrestial minerals. Karr C Jr (ed) Academic Press, New York

  35. Widom B (1967) Intermolecular forces and the nature of the liquid stale. Science. 157:375–382

Download references

Author information

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Lasaga, A.C., Gibbs, G.V. Quantum mechanical potential surfaces and calculations on minerals and molecular clusters. Phys Chem Minerals 16, 29–41 (1988). https://doi.org/10.1007/BF00201327

Download citation

Keywords

  • Silicate
  • Mineral Resource
  • Material Processing
  • Dynamical Property
  • Potential Surface