Controlling Exciton Propagation in Organic Crystals through Strong Coupling to Plasmonic Nanoparticle Arrays
Berghuis, A. M., Tichauer, R. H., de Jong, L. M. A., Sokolovskii, I., Bai, P., Ramezani, M., Murai, S., Groenhof, G., & Gómez Rivas, J. (2022). Controlling Exciton Propagation in Organic Crystals through Strong Coupling to Plasmonic Nanoparticle Arrays. ACS Photonics, 9(7), 2263-2272. https://doi.org/10.1021/acsphotonics.2c00007
Published inACS Photonics
© 2022 the Authors
Exciton transport in most organic materials is based on an incoherent hopping process between neighboring molecules. This process is very slow, setting a limit to the performance of organic optoelectronic devices. In this Article, we overcome the incoherent exciton transport by strongly coupling localized singlet excitations in a tetracene crystal to confined light modes in an array of plasmonic nanoparticles. We image the transport of the resulting exciton–polaritons in Fourier space at various distances from the excitation to directly probe their propagation length as a function of the exciton to photon fraction. Exciton–polaritons with an exciton fraction of 50% show a propagation length of 4.4 μm, which is an increase by 2 orders of magnitude compared to the singlet exciton diffusion length. This remarkable increase has been qualitatively confirmed with both finite-difference time-domain simulations and atomistic multiscale molecular dynamics simulations. Furthermore, we observe that the propagation length is modified when the dipole moment of the exciton transition is either parallel or perpendicular to the cavity field, which opens a new avenue for controlling the anisotropy of the exciton flow in organic crystals. The enhanced exciton–polariton transport reported here may contribute to the development of organic devices with lower recombination losses and improved performance. ...
PublisherAmerican Chemical Society
Publication in research information system
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Related funder(s)Academy of Finland
Funding program(s)Academy Project, AoF
Additional information about fundingThis research is funded by the Innovational Research Incentives Scheme of the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO; Vici Grant 680-47-628) and the Academy of Finland (Grant 323996).
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