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Design principle for increasing charge mobility of π-conjugated polymers using regularly localized molecular orbitals.

Terao J, Wadahama A, Matono A, Tada T, Watanabe S, Seki S, Fujihara T, Tsuji Y - Nat Commun (2013)

Bottom Line: 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.

View Article: PubMed Central - PubMed

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

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.

No MeSH data available.


Syntheses of linear and zigzag IMWs 9 and 10.Complete experimental details and characterization are supplied in the Supplementary Methods section.
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f3: Syntheses of linear and zigzag IMWs 9 and 10.Complete experimental details and characterization are supplied in the Supplementary Methods section.

Mentions: A defect-free linear IMW with a para-poly(phenylene–ethynylene) (para-PPE) backbone was synthesized as a reference polymer via the Sonogashira copolymerization of 5 with 1,4-diethynylbenzene. Sonogashira copolymerization of 8 with 1,3-diiodobenzene yielded twisted IMW 10 containing three PE units between the meta-junctions (Fig. 3).


Design principle for increasing charge mobility of π-conjugated polymers using regularly localized molecular orbitals.

Terao J, Wadahama A, Matono A, Tada T, Watanabe S, Seki S, Fujihara T, Tsuji Y - Nat Commun (2013)

Syntheses of linear and zigzag IMWs 9 and 10.Complete experimental details and characterization are supplied in the Supplementary Methods section.
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC3644079&req=5

f3: Syntheses of linear and zigzag IMWs 9 and 10.Complete experimental details and characterization are supplied in the Supplementary Methods section.
Mentions: A defect-free linear IMW with a para-poly(phenylene–ethynylene) (para-PPE) backbone was synthesized as a reference polymer via the Sonogashira copolymerization of 5 with 1,4-diethynylbenzene. Sonogashira copolymerization of 8 with 1,3-diiodobenzene yielded twisted IMW 10 containing three PE units between the meta-junctions (Fig. 3).

Bottom Line: 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.

View Article: PubMed Central - PubMed

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

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.

No MeSH data available.