title: Design principle for increasing charge mobility of π-conjugated polymers using regularly localized molecular orbitals.
abstract: The feasibility of using π-conjugated polymers as next-generation electronic materials is extensively studied; however, their charge mobilities are lower than those of inorganic materials. Here we demonstrate a new design principle for increasing the intramolecular charge mobility of π-conjugated polymers by covering the π-conjugated chain with macrocycles and regularly localizing π-molecular orbitals to realize an ideal orbital alignment for charge hopping. Based on theoretical predictions, insulated wires containing meta-junctioned poly(phenylene-ethynylene) as the backbone units were designed and synthesized. The zigzag wires exhibited higher intramolecular charge mobility than the corresponding linear wires. When the length of the linear region of the zigzag wires was increased to 10 phenylene-ethynylene units, the intramolecular charge mobility increased to 8.5 cm(2) V(-1) s(-1). Theoretical analysis confirmed that this design principle is suitable for obtaining ideal charge mobilities in π-conjugated polymer chains and that it provides the most effective pathways for inter-site hopping processes.
authors.affiliation: Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan. terao@scl.kyoto-u.ac.jp
authors.forename: Jun
authors.initials: J
authors.lastname: Terao
authors.forename: Akihisa
authors.initials: A
authors.lastname: Wadahama
authors.forename: Akitoshi
authors.initials: A
authors.lastname: Matono
authors.forename: Tomofumi
authors.initials: T
authors.lastname: Tada
authors.forename: Satoshi
authors.initials: S
authors.lastname: Watanabe
authors.forename: Shu
authors.initials: S
authors.lastname: Seki
authors.forename: Tetsuaki
authors.initials: T
authors.lastname: Fujihara
authors.forename: Yasushi
authors.initials: Y
authors.lastname: Tsuji