title: 25th anniversary article: high-mobility hole and electron transport conjugated polymers: how structure defines function.
abstract: The structural organization of three different families of semicrystalline π-conjugated polymers is reported (poly(3-hexylthiophene) (P3HT), poly[2,6-(4,4-bis-alkyl-4H-cyclopenta-[2,1-b;3,4-b0]-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)](cyclopentadithiophene-benzothiadiazole) (CDT-BTZ) and poly(N,N"-bis-2-octyldodecylnaphtalene-1,4,5,8-bis-dicarboximide-2,6-diyl-alt-5,5-2,2-bithiophene (P(NDI2OD-T2))). These have triggered significant interest for their remarkable charge-transport properties. By performing molecular mechanics/dynamics simulations with carefully re-parameterized force fields, it is illustrated in particular how the supramolecular organization of these conjugated polymers is driven by an interplay between the length and nature of the conjugated monomer unit and the packing of their alkyl side chains, and to what extent it impacts the charge-carrier mobility, as monitored by quantum-chemical calculations of the intermolecular hopping transfer integrals. This Progress Report is concluded by providing generic guidelines for the design of materials with enhanced degrees of supramolecular organization.
authors.affiliation: Laboratory for Chemistry of Novel Materials, University of Mons-UMONS, Place du Parc 20, B-7000, Mons, Belgium.
authors.forename: Yoann
authors.initials: Y
authors.lastname: Olivier
authors.forename: Dorota
authors.initials: D
authors.lastname: Niedzialek
authors.forename: Vincent
authors.initials: V
authors.lastname: Lemaur
authors.forename: Wojciech
authors.initials: W
authors.lastname: Pisula
authors.forename: Klaus
authors.initials: K
authors.lastname: Müllen
authors.forename: Unsal
authors.initials: U
authors.lastname: Koldemir
authors.forename: John R
authors.initials: JR
authors.lastname: Reynolds
authors.forename: Roberto
authors.initials: R
authors.lastname: Lazzaroni
authors.forename: Jérôme
authors.initials: J
authors.lastname: Cornil
authors.forename: David
authors.initials: D
authors.lastname: Beljonne
keywords: charge transport; conjugated polymers; molecular modeling; supramolecular organization