Yang Luo

The coherent interaction between quantum emitters and photonic modes in cavities underlies many of the current strategies aiming at generating and controlling photonic quantum states. A plasmonic nanocavity provides a powerful solution for reducing the effective mode volumes down to nanometre scale, but spatial control at the atomic scale of the coupling with a single molecular emitter is challenging. Here we demonstrate sub-nanometre spatial control over the coherent coupling between a single molecule and a plasmonic nanocavity in close proximity by monitoring the evolution of Fano lineshapes and photonic Lamb shifts in tunnelling electron-induced luminescence spectra. The evolution of the Fano dips allows the determination of the effective interaction distance of ∼1 nm, coupling strengths reaching ∼15 meV and a giant self-interaction induced photonic Lamb shift of up to ∼3 meV. These results open new pathways to control quantum interference and field-matter interaction at the nanoscale.

Abstract Achieving strong coupling between plasmonic oscillators can significantly modulate their intrinsic optical properties. Here, we report the direct observation of ultrafast plasmonic hot electron transfer from an Au grating array to an MoS 2 monolayer in the strong coupling regime between localized surface plasmons (LSPs) and surface plasmon polaritons (SPPs). By means of femtosecond pump-probe spectroscopy, the measured hot electron transfer time is approximately 40 fs with a maximum external quantum yield of 1.65%. Our results suggest that strong coupling between LSPs and SPPs has synergetic effects on the generation of plasmonic hot carriers, where SPPs with a unique nonradiative feature can act as an ‘energy recycle bin’ to reuse the radiative energy of LSPs and contribute to hot carrier generation. Coherent energy exchange between plasmonic modes in the strong coupling regime can further enhance the vertical electric field and promote the transfer of hot electrons between the Au grating and the MoS 2 monolayer. Our proposed plasmonic strong coupling configuration overcomes the challenge associated with utilizing hot carriers and is instructive in terms of improving the performance of plasmonic opto-electronic devices.

Abstract Electrically driven molecular light emitters are considered to be one of the promising candidates as single-photon sources. However, it is yet to be demonstrated that electrically driven single-photon emission can indeed be generated from an isolated single molecule notwithstanding fluorescence quenching and technical challenges. Here, we report such electrically driven single-photon emission from a well-defined single molecule located inside a precisely controlled nanocavity in a scanning tunneling microscope. The effective quenching suppression and nanocavity plasmonic enhancement allow us to achieve intense and stable single-molecule electroluminescence. Second-order photon correlation measurements reveal an evident photon antibunching dip with the single-photon purity down to g (2) (0) = 0.09, unambiguously confirming the single-photon emission nature of the single-molecule electroluminescence. Furthermore, we demonstrate an ultrahigh-density array of identical single-photon emitters.