In this work, we report an optical method for characterizing crystal phases along single-semiconductor III-V nanowires based on the measurement of polarization-dependent second-harmonic generation. This powerful imaging method is based on a per-pixel analysis of the second-harmonic-generated signal on the incoming excitation polarization. The dependence of the second-harmonic generation responses on the nonlinear second-order susceptibility tensor allows the distinguishing of areas of pure wurtzite, zinc blende, and mixed and rotational twins crystal structures in individual nanowires. With a far-field nonlinear optical microscope, we recorded the second-harmonic generation in GaAs nanowires and precisely determined their various crystal structures by analyzing the polar response for each pixel of the images. The predicted crystal phases in GaAs nanowire are confirmed with scanning transmission electron and high-resolution transmission electron measurements. The developed method of analyzing the nonlinear polar response of each pixel can be used for an investigation of nanowire crystal structure that is quick, sensitive to structural transitions, nondestructive, and on-the-spot. It can be applied for the crystal phase characterization of nanowires built into optoelectronic devices in which electron microscopy cannot be performed (for example, in lab-on-a-chip devices). Moreover, this method is not limited to GaAs nanowires but can be used for other nonlinear optical nanostructures.
High-quality crystals without inversion symmetry are the conventional platform to achieve optical frequency conversion via three wave-mixing. In bulk crystals, efficient wave-mixing relies on phase-matching configurations, while at the micro-and nanoscale it requires resonant mechanisms that enhance the nonlinear light-matter interaction. These strategies commonly result in wavelength-specific performances and narrowband applications. Disordered photonic materials, made up of a random assembly of optical nonlinear crystals, enable a broadband tunability in the random quasi-phase-matching (RQPM) regime and do not require high-quality materials. Here, we combine resonances and disorder by implementing RQPM in Mie-resonant spheres of a few microns realized by the bottom-up assembly of barium titanate nano-crystals. The measured second harmonic generation (SHG) reveals a combination of broadband and resonant wave mixing, in which Mie resonances drive and enhance the SHG, while the disorder keeps the phase-matching conditions relaxed. This new phase-matching regime can be described by a random walk in the SHG complex plane whose step lengths depend on the local field enhancement within the micro-sphere. Our nano-crystal assemblies provide new opportunities for tailored phase-matching at the micro-scale, beyond the coherence length of the bulk crystal. They can be adapted to achieve frequency conversion from the near-ultraviolet to the infrared ranges, they are low-cost and can cover large surface areas.
In display technologies or data processing, planar and subwavelength free-space components suited for flat photonic devices are needed. Metasurfaces, which shape the optical wavefront within hundreds of nanometers, can provide a solution for thin and portable photonic devices, e.g. as CMOS-compatible modules. While conventional electro-optic modulators are inconvenient to operate in free space configurations, its principle can largely be applied to the development of active metasurfaces with the prospect of modulation speeds up to the GHz region. Here, we use this concept to realize fast and continuous modulation of light at low voltage and MHz speed with a lithium niobate metasurface tuned by the linear electro-optic effect. Furthermore, we exploit the resonance in the visible to enhance the modulation of the transmitted light by two orders of magnitude, namely by a factor of 80, compared to the unstructured substrate. This proof-ofconcept work is a first important step towards the use of lithium niobate metasurfaces for free space modulation.
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