Ab initio molecular dynamics simulation of Na-doped aluminosilicate glasses and glass-water interaction

The structure and properties of sodium aluminosilicate (NAS) glasses are investigated using ab initio molecular dynamics and density functional calculations. Four NAS glass models of about 700 atoms with composition (SiO2)(0.6)(Al2O3)(0.4-x)(Na2O)(x) with Na/Al ratio R = 0.0, 0.5, 1.0 and 1.5 are constructed corresponding to x = 0, 0.135, 0.20 and 0.24. Detailed information on network coordination, electronic structure, interatomic bonding and partial charge distribution, mechanical and optical properties of these models are presented and fully analyzed. The structural details for each R are discussed in terms of short- and intermediate-range order manifested in the coordination number, atomic pair and bond angle distributions. It is shown that the mechanical strength of NAS glasses decreases with increasing Na content, indicating that pure aluminosilicate glass is stronger than the alkali-doped glasses. We use the novel concept of total bond order density to characterize the internal cohesion of the NAS glasses. In the case of R = 1 NAS model, 12 water molecules are added to investigate the solvation effect and hydrolysis in NAS glass.