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Confined organization of fullerene units along high polymer chains

Fang, Lei and Liu, Peng and Sveinbjornsson, Benjamin R. and Atahan-Evrenk, Sule and Vandewal, Koen and Osuna, Sílvia and Jiménez-Osés, Gonzalo and Shrestha, Supriya and Giri, Gaurav and Wei, Peng and Salleo, Alberto and Aspuru-Guzik, Alán and Grubbs, Robert H. and Houk, K. N. and Bao, Zhenan (2013) Confined organization of fullerene units along high polymer chains. Journal of Materials Chemistry C, 1 (36). pp. 5747-5755. ISSN 2050-7526. https://resolver.caltech.edu/CaltechAUTHORS:20130925-111830134

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Abstract

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.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1039/c3tc31158aDOIArticle
http://pubs.rsc.org/en/Content/ArticleLanding/2013/TC/c3tc31158aPublisherArticle
ORCID:
AuthorORCID
Liu, Peng0000-0002-8188-632X
Grubbs, Robert H.0000-0002-0057-7817
Houk, K. N.0000-0002-8387-5261
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.
Funders:
Funding AgencyGrant Number
NSFDMR-1006989
NSFCHE-1059084
NSFDMR-08-20484
Defense Advanced Research Projects Agency (DARPA)UNSPECIFIED
Global Climate and Energy Project (GCEP)UNSPECIFIED
Marie Curie FellowshipPIOF-GA-2009-252856
Ministerio de EducaciónEX2010-1063
Issue or Number:36
Record Number:CaltechAUTHORS:20130925-111830134
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20130925-111830134
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:41526
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:25 Sep 2013 20:34
Last Modified:03 Oct 2019 05:49

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