Enhancement of the third-order optical nonlinearity in ZnO/Al2O3 nanolaminates fabricated by atomic layer deposition

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We investigate the third-order optical nonlinearity in ZnO/Al2O3 nanolaminates fabricated by atomic layer deposition and show that the third-order optical nonlinearity can be enhanced by nanoscale engineering of the thin film structure. The grain size of the polycrystalline ZnO film is controlled by varying the thickness of the ZnO layers in the nanolaminate in which thin (∼2 nm) amorphous Al2O3 layers work as stopping layers for ZnO crystal growth. Nanoscale engineering enables us to achieve a third harmonic generated signal enhancement of ∼13 times from the optimized nanolaminate structure compared to a ZnO reference film of comparable thickness.