A Self‐Assembled Homochiral Radical Cage with Paramagnetic Behaviors

Abstract Condensation of an inherently C 3 ‐symmetric polychlorotriphenylmethyl (PTM) radical trisaldehyde with tris(2‐aminoethyl)amine (TREN) yields a [4+4] tetrahedral radical cage as a racemic pair of homochiral enantiomers in 75 % isolated yield. The structure was characterized by X‐ray crystallography, confirming the homochirality of each cage framework. The homochirality results from intramolecular [CH⋅⋅⋅π] and hydrogen‐bonding interactions within the cage framework. The four PTM radicals in a cage undergo weak through‐space coupling. Magnetic measurements demonstrated that each cage bears 3.58 spins.