Aluminum for nonlinear plasmonics: Resonance-driven polarized luminescence of Al, Ag, and Au nanoantennas

Resonant optical antennas are ideal for nanoscale nonlinear optical interactions due to their inherent strong local field enhancement. Indeed second- and third-order nonlinear response of gold nanoparticles has been reported. Here we compare the on- and off-resonance properties of aluminum, silver, and gold nanoantennas, by measuring two-photon photoluminescence (TPPL). Remarkably, aluminum shows 2 orders of magnitude higher luminescence efficiency than silver or gold. Moreover, in striking contrast to gold, the aluminum emission largely preserves the linear incident polarization. Finally, we show the systematic resonance control of two-photon excitation and luminescence polarization by tuning the antenna width and length independently. Furthermore, we analyze this tuning of the polarization with the rod dimensions by measuring the angular emission of TPPL via back focal plane imaging. Our findings point to aluminum as a promising metal for nonlinear plasmonics.