Enhancement of the internal quantum efficiency in strongly coupled P3HT-C60 organic photovoltaic cells using Fabry-Perot cavities with varied cavity confinement.

The short exciton diffusion length in organic semiconductors results in a strong dependence of the conversion efficiency of organic photovoltaic (OPV) cells on the morphology of the donor-acceptor bulk-heterojunction blend. Strong light-matter coupling provides a way to circumvent this dependence by combining the favorable properties of light and matter via the formation of hybrid exciton-polaritons. By strongly coupling excitons in P3HT-C60 OPV cells to Fabry-Perot optical cavity modes, exciton-polaritons are formed with increased propagation lengths. We exploit these exciton-polaritons to enhance the internal quantum efficiency of the cells, determined from the external quantum efficiency and the absorptance. Additionally, we find a consistent decrease in the Urbach energy for the strongly coupled cells, which indicates the reduction of energetic disorder due to the delocalization of exciton-polaritons in the optical cavity.

Controlling Exciton Propagation in Organic Crystals through Strong Coupling to Plasmonic Nanoparticle Arrays.

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.