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Charge-transfer complexes. NH/sub 3/--O/sub 3/, NH/sub 3/--SO/sub 2/, and N(CH/sub 3/)/sub 3/--SO/sub 2/

Journal Article · · J. Am. Chem. Soc.; (United States)
DOI:https://doi.org/10.1021/ja00440a027· OSTI ID:7232170

The donor--acceptor complex between trimethylamine and sulfur dioxide is the strongest (in terms of its dissociation energy to N(CH/sub 3/)/sub 3/ plus SO/sub 2/) such complex yet to be studied experimentally in the gas phase. Ab initio self-consistent-field theory has been applied to this and two related complexes, NH/sub 3/O/sub 3/ and NH/sub 3/SO/sub 2/. Minimum basis sets were used for all three complexes, while for NH/sub 3/SO/sub 2/ two considerably larger sets (double zeta and double zeta plus sulfur d functions) were employed. The equilibrium structure of these complexes was predicted by an investigation of many points on the respective potential energy surface. To a surprising degree, the O/sub 3/ or SO/sub 2/ molecule is found to lie in a plane nearly perpendicular to ttthe amine C/sub 3v/ axis. Further, the central atom in O/sub 3/ and SO/sub 2/ is predicted to lie only slighty off the amine C/sub 3v/ axis. With these guidelines, the prediction of further structures of this type essentially reduces a one-dimensional search for the central atom-N distance. Using a minimum basis set, the three predicted binding energies at 2.24, 5.00, and 4.06 kcal/mole. Using the double zeta basis set the NH/sub 3/--SO/sub 2/ dissociation energy is increased to 10.40 kcal/mole. When a set of sulfur d functions is added to the latter set, the binding energy becomes 9.30 kcal/mole in the absence of geometry reoptimization.

Research Organization:
Univ. of California, Berkeley
OSTI ID:
7232170
Journal Information:
J. Am. Chem. Soc.; (United States), Journal Name: J. Am. Chem. Soc.; (United States) Vol. 98:24; ISSN JACSA
Country of Publication:
United States
Language:
English