Lasing of moiré trapped MoSe2/WSe2 interlayer excitons coupled to a nanocavity.

We report lasing of moiré trapped interlayer excitons (IXs) by integrating a pristine hBN-encapsulated MoSe2/WSe2 heterobilayer into a high-Q (>104) nanophotonic cavity. We control the cavity-IX detuning using a magnetic field and measure their dipolar coupling strength to be 78 ± 4 micro-electron volts, fully consistent with the 82 micro-electron volts predicted by theory. The emission from the cavity mode shows clear threshold-like behavior as the transition is tuned into resonance with the cavity. We observe a superlinear power dependence accompanied by a narrowing of the linewidth as the distinct features of lasing. The onset and prominence of these threshold-like behaviors are pronounced at resonance while weak off-resonance. Our results show that a lasing transition can be induced in interacting moiré IXs with macroscopic coherence extending over the length scale of the cavity mode. Such systems raise interesting perspectives for low-power switching and synaptic nanophotonic devices using two-dimensional materials.

Coherent Phonons in van der Waals MoSe2/WSe2 Heterobilayers.

The increasing role of two-dimensional (2D) devices requires the development of new techniques for ultrafast control of physical properties in 2D van der Waals (vdW) nanolayers. A special feature of heterobilayers assembled from vdW monolayers is femtosecond separation of photoexcited electrons and holes between the neighboring layers, resulting in the formation of Coulomb force. Using laser pulses, we generate a 0.8 THz coherent breathing mode in MoSe2/WSe2 heterobilayers, which modulates the thickness of the heterobilayer and should modulate the photogenerated electric field in the vdW gap. While the phonon frequency and decay time are independent of the stacking angle between the MoSe2 and WSe2 monolayers, the amplitude decreases at intermediate angles, which is explained by a decrease in the photogenerated electric field between the layers. The modulation of the vdW gap by coherent phonons enables a new technology for the generation of THz radiation in 2D nanodevices with vdW heterobilayers.

Coupling of MoS_{2} Excitons with Lattice Phonons and Cavity Vibrational Phonons in Hybrid Nanobeam Cavities.

We report resonant Raman spectroscopy of neutral excitons X^{0} and intravalley trions X^{-} in hBN-encapsulated MoS_{2} monolayer embedded in a nanobeam cavity. By temperature tuning the detuning between Raman modes of MoS_{2} lattice phonons and X^{0}/X^{-} emission peaks, we probe the mutual coupling of excitons, lattice phonons and cavity vibrational phonons. We observe an enhancement of X^{0}-induced Raman scattering and a suppression for X^{-}-induced, and explain our findings as arising from the tripartite exciton-phonon-phonon coupling. The cavity vibrational phonons provide intermediate replica states of X^{0} for resonance conditions in the scattering of lattice phonons, thus enhancing the Raman intensity. In contrast, the tripartite coupling involving X^{-} is found to be much weaker, an observation explained by the geometry-dependent polarity of the electron and hole deformation potentials. Our results indicate that phononic hybridization between lattice and nanomechanical modes plays a key role in the excitonic photophysics and light-matter interaction in 2D-material nanophotonic systems.

Unveiling the Zero-Phonon Line of the Boron Vacancy Center by Cavity-Enhanced Emission.

Negatively charged boron vacancies (VB-) in hexagonal boron nitride (hBN) exhibit a broad emission spectrum due to strong electron-phonon coupling and Jahn-Teller mixing of electronic states. As such, the direct measurement of the zero-phonon line (ZPL) of VB- has remained elusive. Here, we measure the room-temperature ZPL wavelength to be 773 ± 2 nm by coupling the hBN layer to the high-Q nanobeam cavity. As the wavelength of cavity mode is tuned, we observe a pronounced intensity resonance, indicating the coupling to VB-. Our observations are consistent with the spatial redistribution of VB- emission. Spatially resolved measurements show a clear Purcell effect maximum at the midpoint of the nanobeam, in accord with the optical field distribution of the cavity mode. Our results are in good agreement with theoretical calculations, opening the way to using VB- as cavity spin-photon interfaces.

Nonlocal Exciton-Photon Interactions in Hybrid High-Q Beam Nanocavities with Encapsulated MoS_{2} 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 nonlocal interactions of "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 stems 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 nonmonotonic temperature dependence of the cavity-trion interaction strength, consistent with the nonlocal light-matter interactions in which the extent of the center-of-mass (c.m.) wave function is comparable to the cavity mode volume in space. Our approach can be generalized to other optically active 2D materials, opening the way toward harnessing novel light-matter interaction regimes for applications in quantum photonics.

Efficient Optomechanical Mode-Shape Mapping of Micromechanical Devices.

Visualizing eigenmodes is crucial in understanding the behavior of state-of-the-art micromechanical devices. We demonstrate a method to optically map multiple modes of mechanical structures simultaneously. The fast and robust method, based on a modified phase-lock loop, is demonstrated on a silicon nitride membrane and shown to outperform three alternative approaches. Line traces and two-dimensional maps of different modes are acquired. The high quality data enables us to determine the weights of individual contributions in superpositions of degenerate modes.

Charged Exciton Kinetics in Monolayer MoSe2 near Ferroelectric Domain Walls in Periodically Poled LiNbO3.

Monolayer semiconducting transition metal dichalcogenides are a strongly emergent platform for exploring quantum phenomena in condensed matter, building novel optoelectronic devices with enhanced functionalities. Because of their atomic thickness, their excitonic optical response is highly sensitive to their dielectric environment. In this work, we explore the optical properties of monolayer thick MoSe2 straddling domain wall boundaries in periodically poled LiNbO3. Spatially resolved photoluminescence experiments reveal spatial sorting of charge and photogenerated neutral and charged excitons across the boundary. Our results reveal evidence for extremely large in-plane electric fields of ≃4000 kV/cm at the domain wall whose effect is manifested in exciton dissociation and routing of free charges and trions toward oppositely poled domains and a nonintuitive spatial intensity dependence. By modeling our result using drift-diffusion and continuity equations, we obtain excellent qualitative agreement with our observations and have explained the observed spatial luminescence modulation using realistic material parameters.

The lifetime of interlayer breathing modes of few-layer 2H-MoSe2 membranes.

A time-resolved observation of coherent interlayer longitudinal acoustic phonons in thin layers of 2H-MoSe2 is reported. A femtosecond pump-probe technique is used to investigate the evolution of the energy loss of these vibrational modes in a wide selection of MoSe2 flakes with different thicknesses ranging from bilayer up to the bulk limit. By directly analysing the temporal decay of the modes, we can clearly distinguish an abrupt crossover related to the acoustic mean free path of the phonons in a layered system, and the constraints imposed on the acoustic decay channels when reducing the dimensionality. For thicker samples, the main acoustic attenuation mechanism is attributed to the scattering of the acoustic modes with thermal phonons. For samples thinner than ∼20 molecular layers, the predominant damping mechanism is ascribed to the effects of surface asperity. Losses intrinsic to the low dimensionality of single or few layer materials impose critical limitations for their use in optomechanical and optoelectronic devices.