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Nonlinear crystals that have a noncentrosymmetric crystalline structure, such as lithium niobate (LiNbO 3 ) and barium titanate (BaTiO 3 ) exhibit nonzero second-order tensor susceptibilities (χ (2) ) and linear electro-optic coefficients ( r ij ). The constraints associated with top-down nanofabrication methods have led to bottom up approaches to harness the strong nonlinearities and electro-optical properties. Here, we present an overview of photonic assemblies made of randomly oriented noncentrosymmetric nanocrystals via bottom-up fabrication methods. In this configuration, nanocrystals can form objects with tunable dimensions, increased complexity, and a great span of symmetry level, ranging from thin layers to spheres. At the same time, according to their shape, photonic assemblies may support optical modes, that is, Mie or guided, which can tailor linear optical properties and enhance nonlinear and electro-optic responses. As a result, assemblies of noncentrosymmetric nanocrystals can form a disruptive platform to realize photonic integrated devices free of etching process and over large surface areas. Last, we foresee potential applications of noncentrosymmetric nanocrystals in various fields of nano-optics and sensing., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

Nonlinear disordered photonic media (NDPM), composed of a random configuration of noncentrosymmetric crystals, offer a versatile platform to tailor nonlinear optical effects. The second-harmonic generation (SHG) and its random quasi-phase-matching (RQPM) in the multiple scattering regime are still poorly explored. In this work, we bottom-up assemble NDPM in two different geometries by using LiNbO 3 nanocubes as building blocks and investigate both the multiple scattering and the nonlinear properties. We produce disordered slabs with a continuously variable thickness and microspheres with different diameters, which display a remarkable strong light scattering, evidenced by a subwavelength transport mean free path (). We first provide explicit evidence that the SHG power scales linearly with both the thickness of the slab and the volume of the microspheres. These observations generalize the characteristic linear scaling of RQPM power with the volume to the multiple scattering regime and to different sample geometries. Our structures represent a promising platform to investigate the interplay between disorder and optical nonlinear effects., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)