Tailoring the Third-Order Nonlinear Optical Property of a Hybrid Semiconductor Quantum Dot-Metal Nanoparticle: From Saturable to Fano-Enhanced Absorption.

Semiconductor-metal hybrid nanostructures present an exotic class of nonlinear optical materials due to their potential optoelectronic applications. However, most studies to date focus on their total optical responses instead of contributions from individual nonlinear orders. In this Letter, we present a theoretical study on the third-order nonlinear optical absorption of a hybrid colloidal semiconductor quantum dot (SQD)-metal nanoparticle (MNP) system. We develop a novel analytic treatment based on the nonlinear density matrix equation and derive a closed-form expression for the optical susceptibility. Our study identifies the parameter space that governs the system's optical transition from being a saturable absorber to a Fano-enhanced absorber. We attribute this transition to the plasmon-mediated self-interaction of the SQD. The findings provide a valuable guideline for optimized designs of functional nanophotonic devices based on SQD-MNP hybrid structures.