Lorentz Nanoplasmonics for Nonlinear Generation

While past works have suggested that the Lorentz magnetic contribution to second harmonic generation from metal nanostructures is negligible as compared to other terms, here we demonstrate a dominant Lorentz contribution from T-shaped apertures in a gold film. The apertures are designed to have overlapping magnetic and electric near-field intensities at the plasmonic resonance. This gives 65% greater nonlinear generation from the Lorentz term than the sum of the other two terms. We demonstrate this effect experimentally by milling of nanoapertures of different size and orientation in a metal film and measuring their second harmonic generation. Good agreement is seen between the experiments and comprehensive calculations. In the development of highly efficient nonlinear metasurfaces, careful optimization of the Lorentz contribution should be considered in addition to all other contributions. Following the approach of this work, the Lorentz contribution may also be optimized for THz generation.