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Realization of smaller and faster coherent light sources is critically important for the emerging applications in nanophotonics and information technology. Semiconductor lasers are arguably the most suitable candidate for such purposes. However, the minimum size of conventional semiconductor lasers utilizing dielectric optical cavities for sustaining laser oscillation is ultimately governed by the diffraction limit (∼(λ/2n)(3) for three-dimensional (3D) cavities, where λ is the free-space wavelength and n is the refractive index). Here, we demonstrate the 3D subdiffraction-limited laser operation in the green spectral region based on a metal-oxide-semiconductor (MOS) structure, comprising a bundle of green-emitting InGaN/GaN nanorods strongly coupled to a gold plate through a SiO(2) dielectric nanogap layer. In this plasmonic nanocavity structure, the analogue of MOS-type "nanocapacitor" in nanoelectronics leads to the confinement of the plasmonic field into a 3D mode volume of 8.0 × 10(-4) μm(3) (∼0.14(λ/2n)(3)).

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Plasmonic metasurfaces consist of two-dimensional arrays of metallic nanoresonators (plasmonic "metaatoms"), which exhibit collective and tunable resonance properties controlled by electromagnetic near-field coupling. These man-made surfaces can produce a range of unique optical properties unattainable with natural materials. In this review, we focus on the emerging applications of metasurfaces with precisely engineered plasmonic properties for nonlinear optics and surface-enhanced Raman spectroscopy (SERS). In practice, these applications are quite susceptible to material losses and structural imperfections, such as variations in size, shape, periodicity of meta-atoms, and their material states (crystallinity, impurity, and oxidation, etc.). In these aspects, conventional top-down lithographic techniques are facing major challenges due to inherent limitations in intrinsic material properties and material quality introduced during growth, synthesis, and fabrication processes, as well as achievable lithographic resolution. Moreover, they are prohibitively expensive and timeconsuming for fabrication over large areas. Here, we show that colloidal silver crystals (millimeter-sized single-crystalline plates and thiolate-capped nanoparticles) synthesized by solution-based chemical methods are excellent material platforms for the fabrication of high-quality plasmonic metasurfaces. In particular, both top-down (focused ion-beam milling) and bottom-up (centimeter-scale self-assembly) techniques can be exploited to generate uniform and precisely engineered colloidal metasurfaces for broadband tunable (across the full visible range) second-harmonic generation and quantitative SERS at the single-molecule level.