Avalanche multiphoton photoluminescence (AMPL) is observed from coupled Au–Al nanoantennas under intense laser pumping, which shows more than one order of magnitude emission intensity enhancement and distinct spectral features compared with ordinary metallic photoluminescence. The experiments are conducted by altering the incident laser intensity and polarization using a home-built scanning confocal optical microscope. The results show that AMPL originates from the recombination of avalanche hot carriers that are seeded by multiphoton ionization. Notably, at the excitation stage, multiphoton ionization is shown to be assisted by the local electromagnetic field enhancement produced by coupled plasmonic modes. At the emission step, the giant AMPL intensity can be evaluated as a function of the local field environment and the thermal factor for hot carriers, in accordance with a linear relationship between the power law exponent coefficient and the emitted photon energy. The dramatic change in the spectral profile is explained by spectral linewidth broadening mechanisms. This study offers nanospectroscopic evidence of both the potential optical damages for plasmonic nanostructures and the underlying physical nature of light–matter interactions under a strong laser field; it illustrates the significance of the emerging topics of plasmonic-enhanced spectroscopy and laser-induced breakdown spectroscopy.
Hot carrier-mediated avalanche multiphoton photoluminescence from coupled Au–Al nanoantennas
Jiyong Wang, Anne-Laure Baudrion, Jérémie Béal, Anke Horneber, Feng Tang, Jérémy Butet, Olivier J. F. Martin, Alfred J. Meixner, Pierre-Michel Adam, Dai Zhang; Hot carrier-mediated avalanche multiphoton photoluminescence from coupled Au–Al nanoantennas. J. Chem. Phys. 21 February 2021; 154 (7): 074701. https://doi.org/10.1063/5.0032611
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