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Published 2013 | Published
Journal Article Open

Confined organization of fullerene units along high polymer chains


Conductive fullerene (C_60) units were designed to be arranged in one dimensional close contact by locally organizing them with covalent bonds in a spatially constrained manner. Combined molecular dynamics and quantum chemical calculations predicted that the intramolecular electronic interactions (i.e. charge transport) between the pendant C_60 units could be controlled by the length of the spacers linking the C_60 units and the polymer main chain. In this context, C_60 side-chain polymers with high relative degrees of polymerization up to 1220 and fullerene compositions up to 53% were synthesized by ruthenium catalyzed ring-opening metathesis polymerization of the corresponding norbornene-functionalized monomers. UV/vis absorption and photothermal deflection spectra corroborated the enhanced inter-fullerene interactions along the polymer chains. The electron mobility measured for the thin film field-effect transistor devices from the polymers was more than an order of magnitude higher than that from the monomers, as a result of the stronger electronic coupling between the adjacent fullerene units within the long polymer chains. This molecular design strategy represents a general approach to the enhancement of charge transport properties of organic materials via covalent bond-based organization.

Additional Information

© 2013 The Royal Society of Chemistry. Received 16th June 2013; Accepted 15th July 2013. We are grateful to the National Science Foundation (Z. B.: DMR-1006989; K. N. H.: CHE-1059084; A. A.-G.: DMR-08-20484) and Defense Advanced Research Projects Agency (Z. B. & A. A.-G.: QuBE) for Financial support of this research. We are also grateful to the Stanford GCEP initiative (A. A.-G, S. S. and S. A.). S. O. acknowledges the European Community for the postdoctoral fellowship PIOF-GA-2009-252856. G. J.-O. acknowledges the Ministerio de Educación for the postdoctoral fellowship EX2010-1063. We thank the High Performance Technical Computing Center at the Faculty of Arts and Sciences of Harvard University for invaluable support.

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August 19, 2023
October 24, 2023