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Abstract We demonstrate a simple, femtosecond-scale wavelength tunable, subwavelength-thick nanostructure that performs efficient wavelength conversion from the infrared to the ultraviolet. The output wavelength can be tuned by varying the input power of the infrared pump beam and/or relative delay of the control beam with respect to the pump beam, and does not require any external realignment of the system. The nanostructure is made of chalcogenide glass that possesses strong Kerr nonlinearity and high linear refractive index, leading to strong field enhancement at Mie resonances. Although, as many other materials, chalcogenide glasses absorb in the ultraviolet range, fundamental phase-locking mechanism between the pump and the inhomogeneous portion of the third-harmonic signal enables ultraviolet transmission with little or no absorption. 

Abstract Chalcogenide photonics offers unique solutions for a broad range of applications from mid-infrared sensing to integrated, ultrafast, ultrahigh-bandwidth signal processing. However, to date its usage has been limited to the infrared part of the electromagnetic spectrum, thus avoiding ultraviolet and visible ranges due to absorption of chalcogenide glasses. Here, we experimentally demonstrate and report near-infrared to ultraviolet frequency conversion in an As 2 S 3 -based metasurface, enabled by a phase locking mechanism between the pump and the inhomogeneous portion of the third harmonic signal. Due to the phase locking, the inhomogeneous component co-propagates with the pump pulse and encounters the same effective dispersion as the infrared pump, and thus experiences little or no absorption, consequently opening previously unexploited spectral range for chalcogenide glass science and applications, despite the presence of strong material absorption in this range. 

Abstract Structured lights, including beams carrying spin and orbital angular momenta, radially and azimuthally polarized vector beams, as well as spatiotemporal optical vortices, have attracted significant interest due to their unique amplitude, phase front, polarization, and temporal structures, enabling a variety of applications in optical and quantum communications, micromanipulation, and super‐resolution imaging. In parallel, structured optical materials, metamaterials, and metasurfaces consisting of engineered unit cells—meta‐atoms, opened new avenues for manipulating the flow of light and optical sensing. While several studies explored structured light effects on the individual meta‐atoms, their shapes are largely limited to simple spherical geometries. However, the synergy of the structured light and complex‐shaped meta‐atoms has not been fully explored. In this paper, the role of the helical wavefront of Laguerre–Gaussian beams in the excitation and suppression of higher‐order resonant modes inside all‐dielectric meta‐atoms of various shapes, aspect ratios, and orientations, is demonstrated and the excitation of various multipolar moments that are not accessible via unstructured light illumination is predicted. The presented study elucidates the role of the complex phase distribution of the incident light in shape‐dependent resonant scattering, which is of utmost importance in a wide spectrum of applications ranging from remote sensing to spectroscopy.