Plasmonic Cavities and Individual Quantum Emitters in the Strong Coupling Limit

[Image: see text] The interaction of emitters with plasmonic cavities (PCs) has been studied extensively during the past decade. Much of the experimental work has focused on the weak coupling regime, manifested most importantly by the celebrated Purcell effect, which involves a modulation of the spontaneous emission rate of the emitter due to interaction with the local electromagnetic density of states. Recently, there has been a growing interest in studying hybrid emitter-PC systems in the strong-coupling (SC) regime, in which the excited state of an emitter hybridizes with that of the PC to generate new states termed polaritons. This phenomenon is termed vacuum Rabi splitting (VRS) and is manifested in the spectrum through splitting into two bands. In this Account, we discuss SC with PCs and focus particularly on work from our lab on the SC of quantum dots (QDs) and plasmonic silver bowtie cavities. As bowtie structures demonstrate strong electric field enhancement in their gaps, they facilitate approaching the SC regime and even reaching it with just one to a few emitters placed there. QDs are particularly advantageous for such studies, due to their significant brightness and long lifetime under illumination. VRS was observed in our lab by optical dark-field microspectroscopy even in the limit of individual QDs. We further used electron energy loss spectroscopy, a near-field spectroscopic technique, to facilitate measuring SC not only in bright modes but also in subradiant, dark plasmonic modes. Dark modes are expected to live longer than bright modes and therefore should be able to store electromagnetic energy for longer times. Photoluminescence (PL) is another useful observable for probing the SC regime at the single-emitter limit, as shown by several laboratories. We recently used Hanbury Brown and Twiss interferometry to demonstrate the quantum nature of PL from QDs within PCs, verifying that the measurements are indeed from one to three QDs. Further spectroscopic studies of QD-PC systems in fact manifested several surprising features, indicating discrepancies between scattering and PL spectra. These observations pointed to the contribution of multiple excited states. Indeed, using model simulations based on an extended Jaynes–Cummings Hamiltonian, it was found that the involvement of a dark state of the QDs can explain the experimental findings. Given that bright and dark states couple to the cavity with different degrees of coupling strength, the PC affects in a different manner each excitonic state. This yields complex relaxation pathways and interesting dynamics. Future work should allow us to increase the QD-PC coupling deeper into the SC regime. This will pave the way to exciting applications including the generation of single-photon sources and studies of cavity-induced coherent interactions between emitters.