van der Waals Decoration of Ultra-High-Q Silica Microcavities for χ(2)-χ(3) Hybrid Nonlinear Photonics.

Optical nonlinear processes are indispensable in a wide range of applications, including ultrafast lasers, microscopy, and quantum information technologies. Among the diverse nonlinear processes, second-order effects usually overwhelm the higher-order ones, except in centrosymmetric systems, where the second-order susceptibility vanishes to allow the use of the third-order nonlinearity. Here we demonstrate a hybrid photonic platform whereby the balance between second- and third-order susceptibilities can be tuned flexibly. By decorating ultra-high-Q silica microcavities with atomically thin tungsten diselenide, we observe cavity-enhanced second-harmonic generation and sum-frequency generation with continuous-wave excitation at a power level of only a few hundred microwatts. We show that the coexistence of second- and third-order nonlinearities in a single device can be achieved by carefully choosing the size and location of the two-dimensional material. Our approach can be generalized to other types of cavities, unlocking the potential of hybrid systems with controlled nonlinear susceptibilities for novel applications.

Optical Spectroscopy of Single Colloidal CsPbBr3 Perovskite Nanoplatelets.

Optically bright lead halide perovskite nanocrystals of different morphologies ranging from nanocubes to flat nanoplatelets to elongated nanowires have been reported. The morphology of the nanocrystals is expected to affect various properties such as the band edge energy and the electron-hole exchange interaction. However, aside from nanocubes, the investigation of optical properties in the lead halide perovskite nanocrystals of different morphologies at the single emitter level has been lacking. We have performed optical spectroscopy in single CsPbBr3 nanoplatelets and observed single photon emission without blinking. Furthermore, the photoluminescence emission exhibits excitonic fine structure peaks similar to what has been previously observed in nanocubes. Our work stimulates further investigations into the excitonic and quantum optics properties when the lateral size and morphology can be further controlled in lead halide perovskite nanocrystals.

Silicon nitride nanobeam enhanced emission from all-inorganic perovskite nanocrystals.

Optically active perovskite nanocrystals have shown considerable promise for a myriad of applications, such as single photon source, light-emitting diodes and nanophotonics. Coupling those nanocrystals to photonic micro- and nanostructures will offer additional degrees of freedom to manipulate their optical properties. Herein, we demonstrate the coupling of perovskite nanocrystals to a mechanically robust, poly(methyl-methacrylate) (PMMA)-encapsulated silicon nitride nanobeam photonic crystal cavity at room temperature. As determined from the time-resolved photoluminescence decay measurements, we observed enhanced spontaneous emission from the perovskite nanocrystals by a factor of 1.4, consistent with finite difference time domain simulation. In addition, by varying the concentration of the perovskite nanocrystal in the PMMA layer, the effective index of the layer can be modified, allowing us to tune the cavity mode resonance. Our results show that solution-processable perovskite nanocrystals hold a promising prospect for applications such as on-chip light sources, optoelectronic devices and photonic integrated circuits.

Scheme for media conversion between electronic spin and photonic orbital angular momentum based on photonic nanocavity.

Light with nonzero orbital angular momentum (OAM) or twisted light is promising for quantum communication applications such as OAM-entangled photonic qubits. Methods and devices for the conversion of the photonic OAM to photonic spin angular momentum (SAM), as well as for the photonic SAM to electronic SAM transformation are known but the direct conversion between the photonic OAM and electronic SAM is not available within a single device. Here, we propose a scheme which converts photonic OAM to electronic SAM and vice versa within a single nanophotonic device. We employed a photonic crystal nanocavity with an embedded quantum dot (QD) which confines an electron spin as a stationary qubit. The confined spin-polarized electrons could recombine with holes to give circularly polarized emission, which could drive the rotation of the nanocavity modes via the strong optical spin-orbit interaction. The rotating modes then radiate light with nonzero OAM, allowing this device to serve as a transmitter. As this can be a unitary process, the time-reversed case enables the device to function as a receiver. This scheme could be generalized to other systems with a resonator and quantum emitters such as a microdisk and defects in diamond for example. Our scheme shows the potential for realizing an (ultra)compact electronic SAM-photonic OAM interface to accommodate OAM as an additional degree of freedom for quantum information purposes.

A Nanowire-Based Plasmonic Quantum Dot Laser.

Quantum dots enable strong carrier confinement and exhibit a delta-function like density of states, offering significant improvements to laser performance and high-temperature stability when used as a gain medium. However, quantum dot lasers have been limited to photonic cavities that are diffraction-limited and further miniaturization to meet the demands of nanophotonic-electronic integration applications is challenging based on existing designs. Here we introduce the first quantum dot-based plasmonic laser to reduce the cross-sectional area of nanowire quantum dot lasers below the cutoff limit of photonic modes while maintaining the length in the order of the lasing wavelength. Metal organic chemical vapor deposition grown GaAs-AlGaAs core-shell nanowires containing InGaAs quantum dot stacks are placed directly on a silver film, and lasing was observed from single nanowires originating from the InGaAs quantum dot emission into the low-loss higher order plasmonic mode. Lasing threshold pump fluences as low as ∼120 µJ/cm(2) was observed at 7 K, and lasing was observed up to 125 K. Temperature stability from the quantum dot gain, leading to a high characteristic temperature was demonstrated. These results indicate that high-performance, miniaturized quantum dot lasers can be realized with plasmonics.

Finite-Area Membrane Metasurfaces for Enhancing Light-Matter Coupling in Monolayer Transition Metal Dichalcogenides.

Transition metal dichalcogenides (TMDCs) are at the forefront of nanophotonics because of their exceptional optical characteristics. The 2D architecture of TMDCs facilitates efficient light absorption and emission, holding tantalizing potential for next-generation nanophotonic and quantum devices. Yet, the atomic thinness limits their interaction volume with light, affecting light-matter interaction and quantum efficiency. The light coupling in the 2D layered TMDCs can be enhanced by integration with photonic structure, and the metasurfaces supporting bound states in the continuum (BICs) offer strong confinement of optical fields, ideal for coupling with 2D TMDCs. Here, we demonstrate enhanced light-matter coupling by integrating TMDC monolayers, including WSe2 and MoS2, with a finite-area membrane metasurface, leading to amplified and high-quality-factor (Q-factor) spontaneous emission from quasi-BIC-coupled TMDC monolayers. The high-Q-factor emission extends over an area with a scale of a few micrometers while maintaining the high-Q factor across the emission area. Notably, the suspended finite-area membrane metasurface, which is freestanding in air rather than positioned atop a substrate, minimizes radiation loss while enhancing light-matter interaction in the TMDC monolayer. Furthermore, the predominantly in-plane dipole orientation of excitons within TMDC monolayers results in distinctive enhancement behaviors for emission, contingent on the excitation power, when coupled with quasi-BIC modes exhibiting TE and TM resonances. This work introduces a nanophotonic platform for robust coupling of membrane metasurfaces with 2D materials, offering possibilities for developing 2D material-based nanophotonic and quantum devices.

Transient circular dichroism and exciton spin dynamics in all-inorganic halide perovskites.

All-inorganic metal halides perovskites (CsPbX3, X = Br or Cl) show strong excitonic and spin-orbital coupling effects, underpinning spin-selective excitonic transitions and therefore exhibiting great promise for spintronics and quantum-optics applications. Here we report spin-dependent optical nonlinearities in CsPbX3 single crystals by using ultrafast pump-probe spectroscopy. Many-body interactions between spin-polarized excitons act like a pseudo-magnetic field and thus lift the degeneracy of spin states resulting in a photoinduced circular dichroism. Such spontaneous spin splitting between "spin-up" and "spin-down" excitons can be several tens of milli-electron volts under intense excitations. The exciton spin relaxation time is ~20 picoseconds at very low pump fluence, the longest reported in the metal halides perovskites family at room temperature. The dominant spin-flip mechanism is attributed to the electron-hole exchange interactions. Our results provide essential understandings towards realizing practical spintronics applications of perovskite semiconductors.