Vibrational spectroscopic methods were used to study the Si-O bond character in silicates with different complex anions and crystal structures. The following calcium silicates were examined: Ca<sub>3</sub>(SiO<sub>5</sub>), γ-Ca<sub>2</sub>(SiO<sub>4</sub>), β-Ca<sub>2</sub>(SiO<sub>4</sub>), Ca<sub>3</sub>(Si<sub>2</sub>O<sub>7</sub>), Ca(SiO<sub>3</sub>), and Ca(Si<sub>3</sub>O<sub>3</sub>). The band assignments in IR and Raman spectra of these compounds have been deduced mainly from <sup>28</sup>Si-<sup>30</sup>Si and <sup>40</sup>Ca-<sup>44</sup>Ca isotopic shifts. The GF matrix method and molecular approximation for force constant calculations in silicate anions were used. The Si-O bond parameters (bond order, charge distribution, and bond ionicity, etc.) were obtained from calculated force constants. The nature of Si-O bonds with respect to complex anion and crystal structure will be discussed.

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