Abstract
The cause of irreversible temperature changes in the fine structure of radical pairs in potassium hydrogen malonate previously observed by E.S.R. has been examined in detail by ENDOR. The results show that these changes can be attributed to structural relaxations of the stressed molecules following the abstraction of hydrogens by X-rays at 77 K from the methylene carbons. The appearance of different modifications of pairs is then explicable on the basis of symmetry conditions, which change during annealing of the radicals. In addition the ENDOR results demonstrate that the hyperfine interaction in radical pairs differs from the appropriate coupling constant of the corresponding monoradical in virtue of the transferred hyperfine interaction. It is shown that the transferred hyperfine interaction could be a measure for the direct overlap of the unpaired electrons in radical pairs.
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