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Second harmonic generation (SHG) is forbidden from most bulk metals, becausemetals are characterized by a net zero electric-field in equilibrium. Thislimit breaks down when reaching nanoscale dimensions, as have been shown formetallic nano-particles and nano-cavities. Yet, nonlinear response from athree-dimensional (3D) macroscale metallic piece comprising sub-opticalwavelength features remains a challenge for many years. Herein, we introduce alargescale nanoporous metallic network whose building-blocks are assembled intoan effective nonlinear conductive material, with a considerable conversionefficiency in a wide range of optical wavelengths. The high nonlinear responseresults from the network structure having a large surface area on which theinversion symmetry is broken. In addition, because of the 3D structure,hot-spots can be formed also in deeper focal plans of the metallic network, andthus can give rise to coherent addition of the signal. The solid connectivitybetween the nanoscale building-blocks also plays a role, because it forms arobust network which may respond in a collective manner to form very intensehot-spots. Broadband responses of the metallic network are observed both by SHGand cathodoluminescence (CL). The large-scale dimension and generation ofrandomized hot-spots make this 3D metallic network a promising candidate forapplications like photocatalysis, sensing, or in optical imaging as structuredillumination microscopy.

Nanoporous Metallic Network as a Largescale 3D Source of Second Harmonic Light