Crossover from non-thermal to thermal photoluminescence from metals excited by ultrashort light pulses

Abstract

Photoluminescence from metal nanostructures following intense ultrashort illumination is a fundamental aspect of light-matter interactions. Surprisingly, many of its basic characteristics are under ongoing debate. Here, we resolve the majority of these debates by providing the most complete theoretical framework to date that describes this phenomenon, and support it by experimental confirmation. Specifically, we identify aspects of the emission that are characteristic to either non-thermal or thermal emission, in particular, differences in the spectral and electric field-dependence of these two contributions to the emission. Overall, non-thermal emission is characteristic of the early stages of light emission, while the later stages show thermal characteristics. The former dominate only for moderately high illumination intensities for which the electron temperature reached after thermalization is close to room temperature. The theory is then complemented by experimental evidence that demonstrates the novel aspects of our considerations

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