Intramolecular Spin Transfer in a Spiro‐Fused Bis(triarylamine)

Intriguing electronic properties were observed for the radical cation 1+ of a spiro-fused bis(triarylamine). In a new example of intramolecular spin transfer (IST) in organic intervalence systems connected by a non-π-conjugated bridging unit, the as-prepared radical cation 1+ exhibited thermally activated IST. Furthermore, it was found that 1+ decomposes slowly to the tri-p-anisylamine radical cation.