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Register a new userSuppressed Quenching and Strong Coupling of Purcell-Enhanced Single-Molecule Emission in Plasmonic Nanocavities
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An emitter in the vicinity of a metal nanostructure is quenched by its decay through non-radiative channels, leading to the belief in a zone of inactivity for emitters placed within $<$10nm of a plasmonic nanostructure. Here we demonstrate that in tightly-coupled plasmonic resonators forming nanocavities quenching is quenched due to plasmon mixing. Unlike isolated nanoparticles, plasmonic nanocavities show mode hybridization which massively enhances emitter excitation and decay via radiative channels. This creates ideal conditions for realizing single-molecule strong-coupling with plasmons, evident in dynamic Rabi-oscillations and experimentally confirmed by laterally dependent emitter placement through DNA-origami.
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Strong-coupling of monolayer metal dichalcogenide semiconductors with light offers encouraging prospects for realistic exciton devices at room temperature. However, the nature of this coupling depends extremely sensitively on the optical confinement and the orientation of electronic dipoles and fields. Here, we show how plasmon strong coupling can be achieved in compact robust easily-assembled gold nano-gap resonators at room temperature. We prove that strong coupling is impossible with monolayers due to the large exciton coherence size, but resolve clear anti-crossings for 8 layer devices with Rabi splittings exceeding 135 meV. We show that such structures improve on prospects for nonlinear exciton functionalities by at least 10^4, while retaining quantum efficiencies above 50%.
Fabricating nanocavities in which optically-active single quantum emitters are precisely positioned, is crucial for building nanophotonic devices. Here we show that self-assembly based on robust DNA-origami constructs can precisely position single molecules laterally within sub-5nm gaps between plasmonic substrates that support intense optical confinement. By placing single-molecules at the center of a nanocavity, we show modification of the plasmon cavity resonance before and after bleaching the chromophore, and obtain enhancements of $geq4times10^3$ with high quantum yield ($geq50$%). By varying the lateral position of the molecule in the gap, we directly map the spatial profile of the local density of optical states with a resolution of $pm1.5$ nm. Our approach introduces a straightforward non-invasive way to measure and quantify confined optical modes on the nanoscale.
Strong coupling of plasmonic excitations and dipolar emitters, such as organic molecules, have been studied extensively in the last years. The questions whether strong coupling can be achieved with a single molecule only and how this is unambiguously proven are still under debate. A critical issue of plasmonic in contrast to photonic systems is additional excitonic line broadening, which is often neglected when modeling such systems. This has led to too optimistic design predictions or incorrect interpretation of ambiguous experimental data, for example in models relying on Maxwell solvers without self-consistent incorporation of line broadening effects. In this paper, we present a heuristic modeling approach for strongly coupled systems based on plasmonic nanoparticles and dipolar emitters that accounts for such broadening and elucidates on recent experiments with single emitters. We explicitly focus on a clear and intuitive classical description that utilizes well-established methods, easy to use within typical Maxwell solvers. The heuristic model (i) provides experimentally relevant numbers like emitter densities and spectra (ii) allows to discriminate systems, which can reach the strong coupling regime from those, which can not (iii) allows to identify optimization routes and (iv) nicely matches with experimental findings. In particular, we employ an approach related to quasi normal modes and extinction simulations where the excitonic system is represented by a frequency dependent permittivity. As examples, we investigate two configurations with many, but also single emitters, which have been studied in recent experiments.
Large coupling strengths in exciton-photon interactions are important for quantum photonic network, while strong cavity-quantum-dot interactions have been focused on s-shell excitons with small coupling strengths. Here we demonstrate strong interactions between cavities and p-shell excitons with a great enhancement by the textit{in situ} wave-function control. The p-shell excitons are demonstrated with much larger wave-function extents and nonlocal interactions beyond the dipole approximation. Then the interaction is tuned from the nonlocal to local regime by the wave-function shrinking, during which the enhancement is obtained. A large coupling strength of $210 mumathrm{eV}$ has been achieved, indicating the great potential of p-shell excitons for coherent information exchange. Furthermore, we propose a distributed delay model to quantitatively explain the coupling strength variation, revealing the intertwining of excitons and photons beyond the dipole approximation.
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