Electric field-induced high order nonlinearity in plasmonic nanoparticles retrieved with time-dependent density functional theory

The nonlinear response of metallic nanoparticles is obtained from quantum time dependent density functional theory calculations. Without any aprioristic assumption our calculations allow us to identify high-order harmonic generation in canonical plasmonic structures such as spherical single particles and dimers. Furthermore, we demonstrate that under currently available experimental conditions, the application of an external polarizing field to the nanoparticles allows to actively control even-order harmonic generation in otherwise symmetry forbidden situations. Our quantum calculations provide quantitative access to the high-order response of metallic nanoantennas, which is of utmost importance in the design, control, and exploitation of optoelectronic devices as well as in the generation of extreme ultraviolet radiation.J.A. acknowledges financial support from the Department of Education of the Basque Government through Project IT756/13 for consolidated groups, Project FIS2016-80174-P from the Spanish Ministry of Economy and Competitiveness, and Federal Grant 70NANB15H321 from the National Institute of Standards and Technology (NIST). R.E. acknowledges support from the Fellows Gipuzkoa program of the Gipuzkoako Foru Aldundia through FEDER funds “Una manera de hacer Europa”. A.K.K. acknowledges financial support from Project FIS2016-76617-P of the Spanish Ministry of Economy and Competitiveness.Peer Reviewe