Investigation of new plasmonic material platforms with large optical nonlinearity is crucial for the continued development of nonlinear optics and its applications. Here, we report an enhanced second-order nonlinear effect in metallic quantum wells (QWs), where the intersubband transition plays a dominant role. Centrosymmetry in these metallic QWs is broken by forming multilayers with chemically and structurally distinct barrier oxides above and below a metal nanofilm. For Au-based QWs, we show that a large χ(2) around 229.6 pm/V in the near infrared was achieved in an asymmetric metallic QW of SiO2|Au|HfO2 on a fused silica substrate.
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