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Ab initio calculations at the MP2/6-311 G **//MP2/6-311 G** level show that the all-trans, cis-trans and all-cis rotamers of H 2 S 4  are practically of identical energy. Their vibrational wavenumbers are also practically identical and in agreement with the observed infrared and Raman spectra of dissolved H 2 S 4 . On rotation about the central bond of H 2 S 4  the torsional barriers are found to be 32.0 (cis -barrier) and 26.6 kJ mol -1  (trans-barrier). The geometries of the two transition states with τ SSSS  = 0° and 180° can be explained by hyperconjugation between the lone pairs at the terminal sulfur atoms and the σ * molecular orbital of the central bond.

Structures, Energies, Torsional Barriers, and Vibrational Spectra of Three Rotamers of Tetrasulfane, H 2 S 4