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In a systematic study the Se(IV) and Te(IV) dihalides F 2 E(CH 3 )(C 6 F 5 ), Cl 2 E(CH 3 )(C 6 F 5 ) and Br 2 E(CH 3 )(C 6 F 5 ) (E = Se, Te) have been synthesized and their crystal and molecular structures been investigated by X-ray diffraction and computational methods. The solid-state structures of all compounds show significant correlations between the lengths of the E–C1 bond and the intermolecular E···X (X = F, Cl and Br) contacts, indicating the presence of σ-hole interactions. For comparison, the crystal and gas phase (electron diffraction) structures of Se(CH 3 )(C 6 F 5 ) are presented as well. They show very similar structural parameters in both phases. The structures of the single molecules X 2 E(CH 3 )(C 6 F 5 ) have been analyzed by quantum-chemical methods in terms of their surface potentials. They show significant similarities of their molecular electrostatic-potential topologies ( V   s,max ). The magnitude of  V   s,max  correlates with the aggregation pattern.

Solid-state molecular structures of Se(IV) and Te(IV) dihalides X 2 Se(CH 3 )(C 6 F 5 ) and the gas-phase structure of Se(CH 3 )(C 6 F 5 )