The spin and orbital angular momentum (SAM and OAM) of light is providing a new gateway toward high capacity and robust optical communications. While the generation of light with angular momentum is well studied in linear optics, its further integration into nonlinear optical devices will open new avenues for increasing the capacity of optical communications through additional information channels at new frequencies. However, it has been challenging to manipulate the both SAM and OAM of nonlinear signals in harmonic generation processes with conventional nonlinear materials. Here, we report the generation of spin-controlled OAM of light in harmonic generations by using ultrathin photonic metasurfaces. The spin manipulation of OAM mode of harmonic waves is experimentally verified by using second harmonic generation (SHG) from gold meta-atom with 3-fold rotational symmetry. By introducing nonlinear phase singularity into the metasurface devices, we successfully generate and measure the topological charges of spin-controlled OAM mode of SHG through an on-chip metasurface interferometer. The nonlinear photonic metasurface proposed in this work not only opens new avenues for manipulating the OAM of nonlinear optical signals but also benefits the understanding of the nonlinear spin-orbit interaction of light in nanoscale devices.

In recent years, surface-enhanced Raman scattering (SERS) of a molecule/metal-semiconductor hybrid system has attracted considerable interest and regarded as the synergetic contribution of the electromagnetic and chemical enhancements from the incorporation of noble metal into semiconductor nanomaterials. However, the underlying mechanism is still to be revealed in detail. Herein, we report an irreversible accumulated SERS behavior induced by near-infrared (NIR) light irradiating on a 4-mercaptobenzoic acid linked with silver and silver-doped titanium dioxide (4MBA/Ag/Ag-doped TiO 2) hybrid system. With increasing irradiation time, the SERS intensity of 4MBA shows an irreversible exponential increase, and the Raman signal of the Ag/Ag-doped TiO 2 substrate displays an exponential decrease. A microscopic understanding of the time-dependent SERS behavior is derived based on the microanalysis of the Ag/Ag-doped TiO 2 nanostructure and the molecular dynamics, which is attributed to three factors: (1) higher crystallinity of Ag/Ag-doped TiO 2 substrate; (2) photo-induced charge transfer; (3) chargeinduced molecular reorientation.

Frequency upconversion of Er3+ in alkali bismuth gallate glasses have been investigated. The upconversion mechanisms are discussed, and the dominant mechanisms are excited state absorption for the H11/22→I15/24 and S3/24→I15/24 transitions, and energy transfer upconversion for the F9/24→I15/24 transition. Intense green (around 525–550 nm) and red (around 660 nm) emission bands were observed under 800 nm excitation. At a pump intensity of 15.6 W/cm2, frequency upconversion efficiencies of 2.1×10−2 and 4.8×10−3 were obtained for the green and red emissions, respectively. The results are the highest among doped oxide glasses, and are comparable to those reported for Er3+/Yb3+ codoped fluoride glasses.

Using CMOS-compatible Pd catalysts, we demonstrated the formation of high-mobility ⟨111⟩-oriented GaSb nanowires (NWs) via vapor-solid-solid (VSS) growth by surfactant-assisted chemical vapor deposition through a complementary experimental and theoretical approach. In contrast to NWs formed by the conventional vapor-liquid-solid (VLS) mechanism, cylindrical-shaped PdGa catalytic seeds were present in our Pd-catalyzed VSS-NWs. As solid catalysts, stoichiometric PdGa was found to have the lowest crystal surface energy and thus giving rise to a minimal surface diffusion as well as an optimal in-plane interface orientation at the seed/NW interface for efficient epitaxial NW nucleation. These VSS characteristics led to the growth of slender NWs with diameters down to 26.9 ± 3.5 nm. Over 95% high crystalline quality NWs were grown in ⟨111⟩ orientation for a wide diameter range of between 10 and 70 nm. Back-gated field-effect transistors (FETs) fabricated using the Pd-catalyzed GaSb NWs exhibit a superior peak hole mobility of ∼330 cm V s, close to the mobility limit for a NW channel diameter of ∼30 nm with a free carrier concentration of ∼10 cm. This suggests that the NWs have excellent homogeneity in phase purity, growth orientation, surface morphology and electrical characteristics. Contact printing process was also used to fabricate large-scale assembly of Pd-catalyzed GaSb NW parallel arrays, confirming the potential constructions and applications of these high-performance electronic devices.

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