“…As a wellâknown class of organic dications with excellent redox behavior, viologens ( N , N â˛âdisubstituted 4,4â˛âbipyridinium) have attracted great interests due to their wide applications such as solar energy storage,12 electrochromic display devices,13 organic electrical conductors,14 construction of supramolecular systems and charge transfer materials 15. On the other hand, viologens can also be used as the electron accepters to hybridize with the corresponding electron donors (including halides,16,17 ferrocyanides,18 carboxylate anions,19 amines,20 phenols and arenas21,22) to assemble charge transfer complexes with versatile structural chemistry and optoelectronic properties. Up to date, the simplest methyl viologen, 1,1â˛âdimethylâ4,4â˛âdipyridinium ( M V 2+ ), has been widely studied,23â25 other viologen such as benzyl viologen (BV 2+ ), which possess larger conjugated systems, have been less explored 26,27.…”