Vibration Frequencies of Mg3Al2Si3O12 Pyrope. An ab Initio Study with the CRYSTAL Code
- 11 March 2005
- journal article
- research article
- Published by American Chemical Society (ACS) in The Journal of Physical Chemistry B
- Vol. 109 (13) , 6146-6152
Abstract
The vibrational spectrum of Mg3Al2Si3O12 pyrope is calculated at the Γ point by using the periodic ab initio CRYSTAL program that adopts an all-electron Gaussian-type basis set and the B3LYP Hamiltonian. The full set of frequencies (17 IR active, 25 RAMAN active, 55 silent modes) is calculated. The effect of the basis set and of the computational parameters on the calculated frequencies is discussed. It is shown that the mean absolute difference with respect to the experimental IR and RAMAN data is as small as 6 and 8 cm-1, respectively. The IR and RAMAN modes are fully characterized by various tools such as isotopic substitution, direct inspection of the eigenvectors, and graphical representation. The present calculation permits to clarify some of the assignment and interpretation problems raised by experiment and previous simulations with force fields.Keywords
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