Effect of morphology on ultrafast free carrier generation in polythiophene:fullerene organic solar cells

Ian A. Howard, Ralf Mauer, Michael Meister, Frédéric Laquai

Research output: Contribution to journalArticlepeer-review

363 Scopus citations


Despite significant study, the precise mechanisms that dictate the efficiency of organic photovoltaic cells, such as charge separation and recombination, are still debated. Here, we directly observe efficient ultrafast free charge generation in the absence of field in annealed poly(3- hexylthiophene):melhanofullerene (P3HT:PCBM). However, we find this process is much less efficient in unannealed and amorphous regiorandom blends, explaining the superior short-circuit current and fill-factor of annealed RR-P3HT:PCBM solar cells. We use transient optical spectroscopy in the visible and near-infrared spectral region covering, but not limited to, the previously unobserved and highly relevant time scale spanning 1 to 100 ns, to directly observe both geminate and nongeminate charge recombination. We find that excitan quenching leads directly (time scale less than 100 fs) to two populations: bound charges and free charges. The former do not lead to photocurrent in a photovoltaic cell; they recombine geminately within 2 ns and are a loss channel. However, the latter can be efficiently extracted in photovoltaic cells. Therefore, we find that the probability of ultrafast free charge formation after exciton quenching directly limits solar cell efficiency. This probability is low in disordered P3HT:PCBM blends but approaches unity in annealed blends.

Original languageEnglish (US)
Pages (from-to)14866-14876
Number of pages11
JournalJournal of the American Chemical Society
Issue number42
StatePublished - Oct 27 2010
Externally publishedYes

ASJC Scopus subject areas

  • General Chemistry
  • Biochemistry
  • Catalysis
  • Colloid and Surface Chemistry


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