Density functional based vibrational study of conformational isomers: Molecular rearrangement of benzofuroxan

by Rauhut, G.; Jarzecki, A. A.; Pulay, P.

The molecular rearrangement of benzofuroxan was studied by comparing calculated and experimental IR spectra, the latter taken before and during the reaction. All calculations were performed at the B3-LYP/6-31G(d) density functional level with a further refinement of the computed force constants done by applying the scaled quantum mechanical force field (SQM) technique. Complete assignments for the IR spectra of benzofuroxan and nitrosobenzene are given. The agreement between computed and experimental spectra is excellent, but in benzofuroxan these spectra are very different from previously calculated data. The conformation of the ortho-dinitrosobenzene intermediate of this tautomeric reaction was identified by modeling a composite IR spectrum of four possible components. It shows good agreement with an experimental spectrum that was obtained after photolysing benzofuroxan in Xe matrix. Knowing the conformation of the intermediate provides insight into the reaction mechanism and allows inferences for the thermal reaction, which could not be clarified conclusively by energetic considerations only.

Journal
Journal of Computational Chemistry
Volume
18
Issue
4
Year
1997
Start Page
489-500
URL
https://dx.doi.org/10.1002/(sici)1096-987x(199703)18:4<489::aid-jcc4>3.0.co;2-p
ISBN/ISSN
1096-987X; 0192-8651
DOI
10.1002/(sici)1096-987x(199703)18:4<489::aid-jcc4>3.0.co;2-p