Because of strong light absorption by metals, it is believed that plasmonic nanostructures cannot be used for generating intensive radiation harmonics in the ultraviolet (UV) spectral range. This work presents results of investigation of nonlinear optical interaction with a single gold nanostructure, the split-hole resonator (SHR) under the state-of-the-art experimentally realized conditions. To realize interaction with all spectral components of a 6 fs laser pulse several multipole plasmon resonances were simultaneously excited in the SHR nanostructure. To the best of our knowledge, this paper reports for the first time a strong nonlinear optical interaction at the frequencies of these resonances that leads to (i) the second harmonic generation, (ii) the third harmonic generation (THG), and (iii) the light generation at mixed frequencies. The THG near field amplitude reaches 0.6% of the fundamental frequency field amplitude, which enables the creation of UV radiation sources with a record high intensity. The UV THG may find many important applications including biomedical ones (such as cancer therapy).
Keywords: Plasmonics; UV radiation; nanoantennas; nonlinear optics; second-harmonic generation; third-harmonic generation.