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  1. Abstract New materials that exhibit strong second-order optical nonlinearities at a desired operational frequency are of paramount importance for nonlinear optics. Giant second-order susceptibilityχ(2)has been obtained in semiconductor quantum wells (QWs). Unfortunately, the limited confining potential in semiconductor QWs causes formidable challenges in scaling such a scheme to the visible/near-infrared (NIR) frequencies for more vital nonlinear-optic applications. Here, we introduce a metal/dielectric heterostructured platform, i.e., TiN/Al2O3epitaxial multilayers, to overcome that limitation. This platform has an extremely highχ(2)of approximately 1500 pm/V at NIR frequencies. By combining the aforementioned heterostructure with the large electric field enhancement afforded by a nanostructured metasurface, the power efficiency of second harmonic generation (SHG) achieved 10−4at an incident pulse intensity of 10 GW/cm2, which is an improvement of several orders of magnitude compared to that of previous demonstrations from nonlinear surfaces at similar frequencies. The proposed quantum-engineered heterostructures enable efficient wave mixing at visible/NIR frequencies into ultracompact nonlinear optical devices. 
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