25th anniversary article: High-mobility hole and electron transport conjugated polymers: How structure defines function

Yoann Olivier, Dorota Niedzialek, Vincent Lemaur, Wojciech Pisula, Klaus Müllen, Unsal Koldemir, John R. Reynolds, Roberto Lazzaroni, Jérôme Cornil, David Beljonne

Research output: Contribution to journalArticlepeer-review


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.

Original languageEnglish
Pages (from-to)2119-2136
Number of pages18
JournalAdvanced materials
Issue number14
Publication statusPublished - 9 Apr 2014
Externally publishedYes


  • charge transport
  • conjugated polymers
  • molecular modeling
  • supramolecular organization

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