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Plasmon-assisted two-photon absorption in a semiconductor quantum dot -- metallic nanoshell composite

Tho-photon absorption holds potential for many practical applications. We theoretically investigate the onset of this phenomenon in a semiconductor quantum dot -- metallic nanoshell composite subjected to a resonant CW excitation. Two-photon absorption in this system may occur in two ways: incoherent -- due to a consecutive ground-to-one-exciton-to-biexciton transition and coherent -- due to a coherent two-photon process, involving the direct ground-to-biexciton transition in the quantum dot. The presence of the nanoshell nearby the quantum dot gives rise to two principal effects: (i) -- renormalization of the applied field amplitude and (ii) -- renormalization of the resonance frequencies and radiation relaxation rates of the quantum dot, both depending on the the quantum dot level populations. We show that in the perturbation regime, when the excitonic levels are only slightly populated, each of these factors may give rise to either suppression or enhancement of the two-photon absorption. The complicated interplay of the two determines the final effect. Beyond the perturbation regime, it is found that the two-photon absorption experiences a drastic enhancement, which occurs independently of the type of excitation, either into the one-exciton resonance or into the two-photon resonance. Other characteristic features of the two-photon absorption of the composite, emerging from the coupling between both nanoparticles, are bistability and self-oscillations.

preprint2021arXivOpen access
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