Thickness Insensitive Nanocavities for 2D Heterostructures using Photonic Molecules

Two-dimensional (2D) heterostructures integrated into nanophotonic cavities have emerged as a promising approach towards novel photonic and opto-electronic devices. However, the thickness of the 2D heterostructure has a strong influence on the resonance frequency of the nanocavity. For a single cavity, the resonance frequency shifts approximately linearly with the thickness. Here, we propose to use the inherent non-linearity of the mode coupling to render the cavity mode insensitive to the thickness of the 2D heterostructure. Based on the couple mode theory, we reveal that this goal can be achieved using either a homoatomic molecule with a filtered coupling or heteroatomic molecules. We perform numerical simulations to further demonstrate the robustness of the eigenfrequency in the proposed photonic molecules. Our results render nanophotonic structures insensitive to the thickness of 2D materials, thus owing appealing potential in energy- or detuning-sensitive applications such as cavity quantum electrodynamics

Probing the Dark Exciton in Monolayer MoS2_2 by Quantum Interference in Second Harmonic Generation Spectroscopy

We report resonant second harmonic generation (SHG) spectroscopy of an hBN-encapsulated monolayer of MoS$_2$. By tuning the energy of the excitation laser, we identify a dark state transition (D) that is blue detuned by +25 meV from the neutral exciton X$^0$. We observe a splitting of the SHG spectrum into two distinct peaks and a clear anticrossing between them as the SHG resonance is tuned through the energy of the dark exciton D. This observation is indicative of quantum interference arising from the strong two-photon light-matter interaction. We further probe the incoherent relaxation from the dark state to the bright excitons, including X$^0$ and localized excitons LX, by the resonant enhancement of their intensities at the SHG-D resonance. The relaxation of D to bright excitons is strongly suppressed on the bare substrate whilst enabled when the hBN/MoS$_2$/hBN heterostructure is integrated in a nanobeam cavity. The relaxation enabled by the cavity is explained by the phonon scattering enhanced by the cavity phononic effects. Our work reveals the two-photon quantum interference with long-lived dark states and enables the control through nanostructuring of the substrate. These results indicate the great potential of dark excitons in 2D-material based nonlinear quantum devices

Selective Exciton-Phonon-Phonon Coupling and Anharmonicity with Cavity Vibrational Phonons and MoS2_2 Lattice Phonons in Hybrid Nanobeam Cavities

We report selective coupling between neutral excitons X$^0$, vibrational phonon modes of a freestanding nanobeam cavity and lattice phonons of a MoS$_2$ monolayer fully encapsulated by hBN. Our experimental findings demonstrate that the cavity vibrational phonons selectively couple to neutral excitons (X$^0$), and the coupling to negatively charged trion (X$^-$) being significantly weaker. We establish this result by studying the lattice temperature induced broadening of exciton linewidths, where the contribution from the X$^0$-cavity phonon coupling is clearly observed while the X$^-$-cavity phonon coupling is not. Furthermore, when the Raman modes of MoS$_2$ lattice phonons A$_{1g}$ and 2LA are tuned into an outgoing resonance with exciton emissions, we observe the X$^0$-cavity phonon-lattice phonon coupling which inherits the characteristics rule the of X$^0$-cavity phonon coupling. As a result, X$^0$-induced Raman scatterings are enhanced, while X$^-$-induced scatterings are suppressed, revealed by the detuning-dependent Raman intensities and the ratio of X$^-$/X$^0$ emission intensities. The phonon anharmonicity from the coupling between cavity vibrational phonons and MoS$_2$ lattice phonons is further demonstrated by the observed Raman linewidth. Such hybrid couplings between materials and nanostructures enable the control of phonon-induced processes in nanophotonic and nanomechanical systems incorporating 2D semiconductors

Non-Local Exciton-Photon Interactions in Hybrid High-Q Beam Nanocavities with Encapsulated MoS2 Monolayers

Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of non-local interactions of \textit{free} trions in pristine hBN/MoS$_2$/hBN heterostructures coupled to single mode (Q $>10^4$) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stem from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS$_2$ monolayer. We observe a non-monotonic temperature dependence of the cavity-trion interaction strength, consistent with the non-local light-matter interactions in which the extent of the center-of-mass wavefunction is comparable to the cavity mode volume in space. Our approach can be generalized to other optically active 2D materials, opening the way towards harnessing novel light-matter interaction regimes for applications in quantum photonics