We demonstrate the fabrication of a three-dimensional (3D) polymer quadratic nonlinear () grating structure. By performing layer-by-layer direct laser writing (DLW) and spin-coating approaches, desired photobleached grating patterns were embedded in the guest–host dispersed-red-1/poly(methylmethacrylate) (DR1/PMMA) active layers of an active-passive alternative multilayer structure through photobleaching of DR1 molecules. Polyvinyl-alcohol and SU8 thin films were deposited between DR1/PMMA layers serving as a passive layer to separate DR1/PMMA active layers. After applying the corona electric field poling to the multilayer structure, nonbleached DR1 molecules in the active layers formed polar distribution, and a 3D grating structure was obtained. The grating structures at different DR1/PMMA nonlinear layers were mapped by laser scanning second harmonic (SH) microscopy, and no cross talk was observed between SH images obtained from neighboring nonlinear layers. The layer- by-layer DLW technique is favorable to fabricating hierarchical 3D polymer nonlinear structures for optoelectronic applications with flexible structural design.
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