Phenalenyl radical is an odd-alternant hydrocarbon radical with a highly symmetric (D_(3h)) structure. The high stability and amphoteric redox nature of this radical have triggered studies on its chemical reactivity, physical properties, and functionalities. The main problem hindering the use of phenalenyl radicals as the molecular components of functional materials is their propensity to σ-dimerization. Challenging issue will lie in understanding the self-association character and also in controlling the molecular overlap motif. This article summarizes our studies on the self-association behavior of phenalenyl radicals.
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