Ab initio calculation of vibrational frequencies and Raman spectra of barium peroxide glass including comparison of tetrahedral BaO_4 with GeO_4 and SiO_4

摘要

We have calculated the vibrational frequencies of clusters of atoms from the first principles by using the density-functional theory in the local density approximation (LDA). We are also able to calculate the electronic binding energy for all of the clusters of atoms from the optimized structure. We have made clusters of Ba_nO_m (n, m = 1-6) and have determined the bond lengths, vibrational frequencies as well as intensities in each case. We find that the peroxide cluster BaO_2 occurs with the O-O vibrational frequency of 836.3 cm~(-1). We also find that a glass network occurs in the material which explains the vibrational frequency of 67 cm~(-1). The calculated values agree with those measured from the Raman spectra of barium peroxide and Ba-B-oxide glass. We have calculated the vibrational frequencies of BaO_4, GeO_4 and SiO_4 each in tetrahedral configuration and find that the vibrational frequencies in these systems depend on the inverse square root of the atomic mass.