Vibrational properties of sodosilicate glasses from first-principles calculations

Dimitrios Kilymis (1) , Simona Ispas (1) , Bernard Hehlen (1) , S. Peuget (2) , Jean-Marc Delaye (2)

1 L2C - Laboratoire Charles Coulomb
2 CEA-DES (ex-DEN) - CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire)

The vibrational properties of three sodosilicate glasses have been investigated in the framework of density functional theory. The pure vibrational density of states has been calculated for all systems and the different vibrational modes have been assigned to specific atoms or structuralunits. It is shown that the Na content affects several vibrational features as the position and intensity of the R band or the mixing of the rocking and bending atomic motions of the Si-O-Si bridges. The calculated Raman spectra have been found to agree with experimental observations and their decomposition indicated the dominant character of the non-bridging oxygen contribution on the spectra, in particular for the high-frequency band, above 800 cm −1 . The decomposition of the high-frequency Raman feature into vibrations of the depolymerized tetrahedra (i.e. Q n -units) has revealed spectral shapes of the partial contributions that cannot be accounted for by simple Gaussians as frequently assumed in the treatment of experimentally obtained Raman spectra.

Domaines: Science des matériaux [cond-mat.mtrl-sci]; Systèmes désordonnés et réseaux de neurones [cond-mat.dis-nn]

Dimitrios Kilymis, Simona Ispas, Bernard Hehlen, S. Peuget, Jean-Marc Delaye. Vibrational properties of sodosilicate glasses from first-principles calculations. Physical Review B, 2019, 99, pp.054209. ⟨10.1103/PhysRevB.99.054209⟩. ⟨hal-02043157⟩