An examination of most of the known crystal structures of TCNQ salts is made in connexion with deter mining the amount of charge transfer. A method based on the bond lengths is shown to provide a sensitive test for determining this important quantity'. The charge distribution between different TCNQ molecules of the same compound can also be deduced. The results obtained are used to correlate the degree of charge with the occurrence of a hydrogen bond. the rotation of C(CN)z groups and the experimental values of dipolar splittings D and E.
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