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Calculated geometries, vibrational spectra, energetics, and electronic properties of fluorinated methanes and silanes

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j100312a021· OSTI ID:5416970
A variety of molecular properties have been calculated for fluorinated methanes and silanes by ab initio molecular orbital theory with large basis sets. Excellent agreement between theory and experiment is found for structural properties and vibrational spectra. Calculated infrared intensities are given for all of the compounds, and agreement with experiment is generally within a factor of 2. A series of isodesmic reactions are presented, and theory and experiment are in excellent agreement for the methanes. The authors use these reactions to calculate ..delta..H/sub f//sup 0/'s of -85.6 +/- 1, -185.7 +/- 1, and -287.7 +/- 1 kcal/mol for SiH/sub 3/F, SiH/sub 2/F/sub 2/, and SiHF/sub 3/, respectively. Good values for these ..delta..H/sub f//sup 0/'s are not available from experiment. Dipole moments, polarizabilites, quadrupole moments, and Mulliken charge distributions are presented. The Mulliken charges show a significant amount of ionic bonding with approx. 1 electron transferred to the fluorines in CH/sub 4/ and 1.5-2.0 electrons transferred to the fluorines in SiF/sub 4/. Large contributions from polarization functions on the central atom are consistent with the large charge transfer to the ligands.
Research Organization:
E.I. du Pont de Nemours and Company, Wilmington, DE
OSTI ID:
5416970
Journal Information:
J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 92:1; ISSN JPCHA
Country of Publication:
United States
Language:
English