Ultrashort laser pulse-induced anti-Stokes photoluminescence of hot electrons in gold nanorods

We report observing anti-Stokes broadband radiation induced in gold nanorods by ultrashort laser pulses. The radiation is in the visible spectral range along with the second harmonic peak. Unlike conventional photoluminescence of metal nanoparticles, the energy of the excitation photons is smaller than the gap between the top of the d band and the Fermi level. Because the gold nanorods are irradiated with a pulse whose time is shorter than the electron–phonon equilibration time in gold, the energy is absorbed by s/p band electrons, creating a temperature difference between the electrons and the lattice, as described by the two-temperature model. Therefore, we identify the origin of the observed radiation as the recombination of hot conduction electrons with the d band holes created by the same ultrashort laser pulse.