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Amidines have found widespread use, but their solution chemistry remains poorly understood. In this work, X‐ray crystallographic and detailed 1D and 2D NMR spectroscopic studies have been performed to elucidate the preferred isomers and their interconversion mechanisms. Amidines are shown to exist as a mixture of E‐syn and Z‐anti isomers in solution and to form dimeric H‐bonded aggregates that are...
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