Nonlinear plasmonics at high temperatures

We solve the Maxwell and heat equations self-consistently for metal nanoparticles under intense continuous wave (CW) illumination. Unlike previous studies, we rely on experimentally-measured data for metal permittivity for increasing temperature and for the visible spectral range. We show that the thermal nonlinearity of the metal can lead to substantial deviations from the predictions of the linear model for the temperature and field distribution and, thus, can explain qualitatively the strong nonlinear scattering from such configurations observed experimentally. We also show that the incompleteness of existing data of the temperature dependence of the thermal properties of the system prevents reaching a quantitative agreement between the measured and calculated scattering data. This modeling approach is essential for the identification of the underlying physical mechanism responsible for the thermo-optical nonlinearity of the metal and should be adopted in all applications of high-temperature nonlinear plasmonics, especially for refractory metals, for both CW and pulsed illumination.