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A simple and efficient ‘one-pot’ methodology was developed to generate a new series of tetrahydro-β-carboline (THBC), tetrahydroisoquinoline (THIQ) and tetrahydrothienopyridine (THTP) derivatives. The key step of the methodology is based on a Pictet–Spengler type cyclization of a reactive N-carbamyliminium ion. This methodology was applied to the synthesis of a library of 32 compounds with potential...