Document Type

Article

Version

Author's Final Manuscript

Publication Title

The Journal of Physical Chemistry A

Volume

110

Publication Date

2006

Abstract

The molecular and crystal structure of 3-(trifluoromethyl)phenanthrene has been determined by X-ray diffraction. The structure of the isolated molecule has been calculated using electronic structure methods at the HF/3-21G, HF/6-31G*, MP2/6-31G* and B3LYP/6-31G* levels. The potential energy surfaces for the rotation of the CF3 group in both the isolated molecule and cluster models for the crystal were computed using electronic structure methods. The barrier height for CF3 rotation in the isolated molecule was calculated to be 0.40 kcal mol-1 at B3LYP/6-311+G**//B3LYP/6-311+G**. The B3LYP/6-31G* calculated CF3 rotational barrier in a 13-molecule cluster based on the X-ray data was found to be 2.6 kcal mol-1. The latter is in excellent agreement with experimental results from the NMR relaxation experiments reported in the companion paper (Beckmann, P. A.; Rosenberg, J.; Nordstrom, K.; Mallory, C. W.; Mallory, F. B. J. Phys. Chem. A 2006, 110, 3947). The computational results on the models for the solid state suggest that the intermolecular interaction between nearest neighbor pairs of CF3 groups in the crystal accounts for roughly 75% of the barrier to rotation in the solid state. This pair is found to undergo cooperative reorientation. We attribute the CF3 reorientational disorder in the crystal as observed by X-ray diffraction to the presence of a pair of minima on the potential energy surface and the effects of librational motion.

DOI

http://pubs.acs.org/doi/abs/10.1021/jp056662y

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