This paper describes the preparation of two tetracations
4a4+ and
4b4+ composed of di(1-azulenyl)methylium units based on a new structural principle of a cyanine-cyanine hybrid for the design ofelectrochromic materials with two color changes. Di- and monocations
5a2+,
5b2+ and
6a+,
6b+ composedof di(1-azulenyl)methylium units were also prepared for the purpose of comparison. The p
KR+ values ofthe tetracations are rather high despite their tetracationic structure, although the stability of these cationsdecreases with the increase of the number of the existing cation units. The cyclic voltammetry (CV) ofthese cations revealed the presumed multielectron redox properties. However, the tetracations did notexhibit the idealized electrochemical behavior, in which subsequent two-electron reduction was presumedas the cyanine-cyanine hybrid, probably due to the less effective electrochemical interaction among thepositive charges. The scope of the creation of the novel polyelectrochromic materials taking the newstructural principle is demonstrated by these examples.