Instabilities in the optical response of a semiconductor quantum dot—metal nanoparticle heterodimer: self-oscillations and chaos

Abstract

We theoretically investigate the nonlinear optical response of a heterodimer comprising a semiconductor quantum dot strongly coupled to a metal nanoparticle. The quantum dot is considered as a three-level ladder system with ground, one-exciton, and bi-exction states. As compared to the case of a two-level quantum dot model, adding the third (bi-exciton) state produces fascinating effects in the optical response of the hybrid system. Specifically, we demonstrate that the system may exhibit picosecond and sub-picosecond self-oscillations and quasi-chaotic behaviour under single-frequency continuous wave excitation. An isolated semiconductor quantum dot does not show such features. The effects originate from competing one-exciton and bi-exciton transitions in the semiconductor quantum dot, triggered by the selfaction of the quantum dot via the metal nanoparticle. The key parameter that governs the phenomena mentioned is the ratio of the self-action strength and the bi-exciton shift. The selfoscillation regime can be achieved in practice, in particular, in a heterodimer comprised of a closely spaced ZnS/ZnSe core-shell quantum dot and a spherical silver nanoparticle. The results may have applications in nanodevices for generating trains of ultrashort optical pulses.