Nonadiabatic multi-step excitation for the blue–green light emission from dye grains induced by the near-infrared optical near-field

Blue–green light emission (wavelength range: 460–520 nm) from coumarin dye grains due to near-infrared excitation (CW, λex=808 nm), based on the nonadiabatic excitation process induced by an optical near-field, was observed. A maximum frequency up-shift of 1.17 eV was confirmed. Based on the excitation intensity dependence, a light emission mechanism originating from a nonadiabatic three-step excitation was confirmed for the first time. The lifetime of the intermediate excited state was approximately 1.1–1.9 ps, and thus realization of frequency up-conversion with a rapid response can be expected.