Abstract
A molecular-level mechanism is proposed for two cases of mechanochemical cocrystallization via halogen bonds. The proposed stepwise mechanism is based on the observation and structural characterization of intermediates that appear in early stages of the reaction. The mechanism arises from the competition of strong and weak intermolecular halogen bonds of the N...I and S...I type and involves the initial formation of finite molecular assemblies, held together via N...I bonds that subsequently polymerize into infinite chains by cross-linking through S...I bonds. This mechanism has been observed in the synthesis of linear as well as zigzag halogen-bonded chain architectures.
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