Impact of Double‐π‐Bridge on Bis(triarylamine)‐Based Organic Mixed‐Valence System: A Case Study of Diaza[1.1](4,4”)ortho‐terphenylophane Radical Cation

A bis(triarylamine) (BTA) radical cation, bridged by two o‐terphenylene moieties, was prepared and characterized to explore the impact of the double‐π‐bridge on the intramolecular charge/spin transfer process in the 2‐site organic mixed‐valence (MV) compound. Spectroscopic analyses on optically and thermally assisted intervalence charge‐transfer (IVCT) processes revealed that the doubly π‐bridging enhanced the charge delocalization between two nitrogen redox‐active centers, whereas the electronic coupling was not so strengthened, in comparison with the singly π‐bridging reference compound.