Metal nanoparticles can strongly enhance such nonlinear optical processes as harmonic generation and multiphoton photoluminescence due to their high electronic polarizabilities, intense optical resonances and high surface-to-volume ratio. Heavily doped semiconductor nanoparticles, such as metal chalcogenides, can also exhibit plasmonic resonances in addition to their excitonic response. Here we describe frequency upconversion in bilayer nanoparticle thin-film structures comprising copper sulfide and gold nanoparticles separated by insulating ligands or thin films when excited by near-infrared femtosecond laser pulses. The surprisingly large third-harmonic signal is due to coherent excitation of the LSPR in both semiconducting and metallic nanoparticles – a mechanism validated by a dipole-dipole model calculation
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