Raman antenna effect from exciton-phonon coupling in organic semiconducting nanobelts

Mao Wang, Yi Gong, Francesc Alzina, Ondrej Svoboda, Belén Ballesteros, Clivia M. Sotomayor Torres, Senbo Xiao, Zhiliang Zhang, Jianying He

    Research output: Contribution to journalArticleResearchpeer-review

    3 Citations (Scopus)

    Abstract

    © 2017 The Royal Society of Chemistry. The highly anisotropic interactions in organic semiconductors together with the soft character of organic materials lead to strong coupling between nuclear vibrations and exciton dynamics, which potentially results in anomalous electrical, optical and optoelectrical properties. Here, we report on the Raman antenna effect from organic semiconducting nanobelts 6,13-dichloropentacene (DCP), resulting from the coupling of molecular excitons and intramolecular phonons. The highly ordered crystalline structure in DCP nanobelts enables the precise polarization-resolved spectroscopic measurement. The angle-dependent Raman spectroscopy under resonant excitation shows that all Raman modes from the skeletal vibrations of DCP molecule act like a nearly perfect dipole antenna IRaman ∝ cos4(θ - 90), with almost zero (maximum) Raman scattering parallel (perpendicular) to the nanobelt's long-axis. The Raman antenna effect in DCP nanobelt is originated from the coupling between molecular skeletal vibrations and intramolecular exciton and the confinement of intermolecular excitons. It dramatically enhances the Raman polarization ratio (ρ =I∥/I⊥ > 25) and amplifies the anisotropy of the angle-dependent Raman scattering (κRaman = Imax/Imin > 12) of DCP nanobelts. These findings have crucial implications for fundamental understanding on the exciton-phonon coupling and its effects on the optical properties of organic semiconductors.
    Original languageEnglish
    Pages (from-to)19328-19336
    JournalNanoscale
    Volume9
    Issue number48
    DOIs
    Publication statusPublished - 28 Dec 2017

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