Continuous-wave multiphoton photoemission from plasmonic nanostars

Abstract Highly nonlinear optical processes require high intensities, typically achieved with ultrashort laser pulses, and hence, they were first observed with the advent of picosecond laser technology. An alternative approach for reaching the required field intensities is offered by localized optical resonances in tailored plasmonic nanostructures, enabling the enhancement of a multitude of nonlinear phenomena. However, so far, plasmon-enhanced high-order nonlinear effects have been restricted to experiments involving short-pulsed and ultrafast laser sources. Here, we demonstrate localized three-photon photoemission from chemically synthesized plasmonic gold nanostars under continuous-wave illumination at sub-MWcm−2 incident intensities. Intensity- and polarization-dependent measurements confirm the nonlinearity of the photoemission process and agree with quantum mechanical calculations of the electron yield from nanostar tips with features smaller than 5 nm, which facilitate local intensity enhancement factors exceeding 1000. Our results open up new avenues for the design of accessible nanoscale coherent electron sources, with potential applications in microscopy, spectroscopy, sensing, and signal processing.