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Ab initio calculations (RHF/6-31G*//6-31G* and MP2/6-31G*//6-31G*) produced the result that methyl isothiocyanate is more stable than methyl thiocyanate by 4.6 kcal/mol and vinyl isothiocyanate is 8.6-8.7 kcal/mol more stable than vinyl thiocyanate. We thank Professor Dr. Ernst-Ulrich Würthwein, Universität Münster, for these calculations.
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