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High intrachain order promotes triplet formation from recombination of long-lived polarons in poly(3-hexylthiophene) J-aggregate nanofibers. | LitMetric

AI Article Synopsis

  • – J-aggregate nanofibers exhibit large quenching depths while H-aggregate nanofibers demonstrate much smaller quenching, indicating that the structural organization of P3HT chains affects PL behavior and triplet formation.
  • – The findings suggest that improving intrachain order in polymer assemblies can influence exciton coupling and control the balance between different spin states, highlighting potential future strategies for

Article Abstract

Photoluminescence (PL) of single poly(3-hexylthiophene) (P3HT) J-aggregate nanofibers (NFs) exhibits strong quenching under intensity-modulated pulsed excitation. Initial PL intensities (I(0)) decay to steady-state levels (ISS) typically within ∼ 1-10 μs, and large quenching depths (I(0)/I(SS) >2) are observed for ∼ 70% of these NFs. Similar studies of polymorphic, H-aggregate type P3HT NFs show much smaller PL quenching depths (I(0)/I(SS) ≤ 1.2). P3HT chains in J-type NF π-stacks possess high intrachain order, which has been shown previously to promote the formation of long-lived, delocalized polarons. We propose that these species recombine nongeminately to triplets on time scales of >1 ns. The identity of triplets as the dominant PL quenchers was confirmed by subjecting NFs to oxygen, resulting in an instantaneous loss of triplet PL quenching (I(0)/I(SS) ∼ 1). The lower intrachain order in H-type NFs, similar to P3HT thin-film aggregates, localizes excitons and polarons, leading to efficient geminate recombination that suppresses triplet formation at longer time scales. Our results demonstrate the promise of self-assembly strategies to control intrachain ordering within multichromophoric polymeric aggregate assemblies to tune exciton coupling and interconversion processes between different spin states.

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Source
http://dx.doi.org/10.1021/nn5040026DOI Listing

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