Fang, LeiLiu, PengSveinbjornsson, Benjamin R.Atahan-Evrenk, SuleVandewal, KoenOsuna, SílviaJiménez-Osés, GonzaloShrestha, SupriyaGiri, GauravWei, PengSalleo, AlbertoAspuru-Guzik, AlanGrubbs, Robert H.Houk, K. N.Bao, Zhenan2014-06-202013Fang, Lei, Peng Liu, Benjamin R. Sveinbjornsson, Sule Atahan-Evrenk, Koen Vandewal, Sílvia Osuna, Gonzalo Jiménez-Osés, et al. 2013. Confined Organization of Fullerene Units Along High Polymer Chains. Journal of Materials Chemistry C 1(36):5747.2050-75262050-7534http://nrs.harvard.edu/urn-3:HUL.InstRepos:12361253Conductive 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.en-USJournal Article2014-06-2010.1039/c3tc31158a