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Micro and Nanostructures

Nonlinear optical response of a strongly-driven quantum dot exciton-biexciton system

Spyridon G. Kosionis, Emmanuel Paspalakis

Published Jan 19, 2023• 8 citations
Publisher
DOI
10.1016/j.micrna.2023.207508

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We report on large optical nonlinear effects induced by coherent interactions between excitons and biexcitons in quantum dots. The absorption spectra in an exciton–biexciton system are measured in InGaAs quantum dots by using single dot spectroscopy. The spectra exhibit unusual shapes that have a transparent region under a strong excitation condition. A pump–probe measurement ensures that the exciton state is erased by a quantum interference effect with exciton and biexciton photoabsorption processes. These results suggest that optical functions such as electromagnetically induced transparency are feasible with excitons and biexcitons in quantum dots.
This study presents a theoretical study of ground-state exciton and biexciton properties in strongly prolate ellipsoidal GaAs quantum dot. Using a variational approach with trial wave functions constructed from single-particle states, we examine the dependence of exciton and biexciton energies on the dot’s geometric parameters. The oscillator strengths of exciton–biexciton transitions are analyzed as functions of the major and minor semiaxes. We further investigate the third-order optical susceptibility near single- and two-photon resonances, elucidating the role of exciton–biexciton interactions. The results show that one-photon resonances dominate the nonlinear response, with contributions exceeding those of two-photon resonances by approximately four orders of magnitude. Absorption coefficients for exciton and biexciton transitions are evaluated for a fixed major semiaxis and varying minor semiaxis, along with the biexciton two-photon absorption coefficient. Finally, we analyze biexciton-induced nonlinear refractive index modulation, which exhibits a sign reversal across resonance and a pronounced peak–dip structure, indicating strong dispersive behavior and significant excitonic phase modulation.
The vectorial four-wave mixing response of an individual strongly confined exciton–biexciton system with fine-structure splitting in a GaAs/AlGaAs quantum dot is measured by dual-polarization heterodyne spectral interferometry. The results are compared with theoretical predictions based on the optical Bloch equations. The system is described by a four-level scheme, which is a model system of the nonlinear excitonic response in low-dimensional semiconductors. We measure its coherence properties and determine the underlying dephasing mechanisms. An impact of the inhomogeneous broadening by spectral wandering on the coherent response is investigated. We further discuss the different four-wave mixing pathways, polarization selection rules, the time-resolved polarization state, the vectorial response in two-dimensional four-wave mixing and ensemble properties.