Abstract
Non‐radiative energy transfer between spatially‐separated molecules in a microcavity can occur when an excitonic state on both molecules are strongly‐coupled to the same optical mode, forming so‐called “hybrid” polaritons. Such energy transfer has previously been explored when thin‐films of different molecules are relatively closely spaced (≈100 nm). In this manuscript, we explore strong‐coupled microcavities in which thin‐films of two J‐aggregated molecular dyes were separated by a spacer layer having a thickness of up to 2 μm. Here, strong light‐matter coupling and hybridisation between the excitonic transition is identified using white‐light reflectivity and photoluminescence emission. We use steady‐state spectroscopy to demonstrate polariton‐mediated energy transfer between such coupled states over “mesoscopic distances”, with this process being enhanced compared to non‐cavity control structures.
Highlights
Our approach, recently proposed in a theoretical work by Balasubrahmaniyam et al.[1] and experimentally confirmed by Georgiou et al.[2] is different from the (N+1) x (N+1) Hamiltonian that we have used previously to describe multimode optical cavities[3]
The model is based on a 3N x 3N Hamiltonian shown in matrix Equation (1) of the manuscript, where there are 3 individual species that can mutually hybridise with N being the number of dispersive optical modes that become resonant with the two excitons
We find that the “conventional” N+2 Hamiltonian model shown in Figure S3b and d fits the experimental data relatively well, we observe a small deviation between experimental and simulation polariton modes, at energetic regions around the exciton energies
Summary
Recently proposed in a theoretical work by Balasubrahmaniyam et al.[1] and experimentally confirmed by Georgiou et al.[2] is different from the (N+1) x (N+1) Hamiltonian that we have used previously to describe multimode optical cavities[3]. We plot the same experimental reflectivity maps shown in the paper (Figure 2a and c) we plot data over a reduced spectral range (550 – 700 nm) and overlay it with the polariton energies extracted from the two different models. At this point, it is apparent from the experimental data that there is a splitting of the polariton mode which is only correctly described by the 3N Hamiltonian model used in Figure S3a (splitting between modes MP4 and UP3). We plot the figure over a more extended wavelength range (between 530 nm to 805 nm), allowing photon mode Γ1 and polariton branch LP1 to be seen
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