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Journal of Applied Physics

Pump-probe optical response of semiconductor quantum dot–metal nanoparticle hybrids

Spyridon G. Kosionis, Emmanuel Paspalakis

Published Dec 14, 2018• 41 citations
Publisher

Abstract

We study optical effects in a hybrid system composed of a semiconductor quantum dot (SQD) and a spherical metal nanoparticle (MNP) that interacts with a weak probe and a strong pump electromagnetic field. We use modified nonlinear density matrix equations for the description of the optical properties of the system and calculate, numerically, the first-order susceptibilities of the SQD, the MNP, and the total hybrid nanostructure of the probe field in the presence of the pump field. We investigate the dependence of the probe absorption and dispersion spectra of the SQD, the MNP, and the total nanostructure on the interparticle distance and the detuning of the pump field, and stress the influence of the MNP contribution to the total optical response. The results we find are explained according to the theory of two distinct metastates, which constitute conjugations of the SQD excitonic and the MNP plasmonic excitations. We also show that the optical response strongly depends on the actual values of the SQD material parameters.

DOI
10.1063/1.5054838

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We study optical effects in a hybrid system composed of a semiconductor quantum dot (SQD) and a spherical metal nanoparticle (MNP) that interacts with a weak probe and a strong pump electromagnetic field. We use modified nonlinear density matrix equations for the description of the optical properties of the system and calculate, numerically, the first-order susceptibilities of the SQD, the MNP, and the total hybrid nanostructure of the probe field in the presence of the pump field. We investigate the dependence of the probe absorption and dispersion spectra of the SQD, the MNP, and the total nanostructure on the interparticle distance and the detuning of the pump field, and stress the influence of the MNP contribution to the total optical response. The results we find are explained according to the theory of two distinct metastates, which constitute conjugations of the SQD excitonic and the MNP plasmonic excitations. We also show that the optical response strongly depends on the actual values of the SQD material parameters.
In the present work, we investigate the modified nonlinear pump-probe optical properties due to the excitonic–plasmonic interaction of a double semiconductor quantum dot (SQD) molecule coupled to a metal nanoparticle (MNP). More specifically, we study the absorption and the dispersion spectra of a weak electromagnetic field in a hybrid structure with two counterparts, a molecule of two coupled SQDs, and a spherical MNP driven by a field of high intensity. We solve the relevant density matrix equations, calculate the first-order optical susceptibility of the probe field in the strong pumping regime, and investigate the way in which the distance between the two counterparts modifies the optical response, for a variety of values of the physical constants of the system, including the pump-field detuning, the tunnelling rate, and the energy separation gap associated with the excited states of the coupled SQDs.
We study optical effects in a hybrid system composed of a semiconductor quantum dot and a spherical metal nanoparticle that interacts with a weak probe electromagnetic field. We use modified nonlinear density matrix equations for the description of the optical properties of the system and obtain a closed-form expression for the linear susceptibilities of the quantum dot, the metal nanoparticle, and the total system. We then investigate the dependence of the susceptibility on the interparticle distance as well as on the material parameters of the hybrid system. We find that the susceptibility of the quantum dot exhibits optical transparency for specific frequencies. In addition, we show that there is a range of frequencies of the applied field for which the susceptibility of the semiconductor quantum dot leads to gain. This suggests that in such a hybrid system quantum coherence can reverse the course of energy transfer, allowing flow of energy from the metallic nanoparticle to the quantum dot. We also explore the susceptibility of the metal nanoparticle and show that it is strongly influenced by the presence of the quantum dot.
The self-Kerr nonlinear optical response of a probe field is investigated in the presence of a near-resonant pump field in coupled metal nanoparticle (MNP)–semiconductor quantum dot (SQD) nanostructures. The study of the spectra is based on the solution of the resulted density matrix equations for the case of a colloidal CdSe-based SQD–(Au)MNP molecule, as well as for an epitaxial SQD structure coupled to an Au nanoparticle. It is demonstrated that below a critical value of the interparticle distance the susceptibility of each distinct component of the structure exhibits a characteristic single-resonance spectrum, whereas above this value, the spectrum has three resonances. This phenomenon can be understood in terms of the theory of exciton–plasmon quantum metastates. In addition, the conditions under which optical transparency occurs with a concurrent positive self-phase-modulation coefficient are also identified.
The optical polarization from a hybrid system including a closely spaced spherical SQD (modeled as a three-level V-type system) and a metal nanoparticle which are considered classically and are connected by the dipole–dipole interaction mechanism is investigated. The interaction between the SQD and the MNP shows an interesting optical response. In the weak probe field regime and MNP nonlocality correction, the absorption spectrum of the hybrid system exhibits an EIT window with two absorption peaks and the plasmon-assisted quantum interference plays an important role in the position and amplitude of these peaks, which are intensely altered by including the nonlocal effects. The probe diffraction grating is created based on the excitons-induced transparency by applying a standing-wave coupling field. The results of this study are useful in numerous areas of all-optical communications.
We theoretically investigated optical third-order nonlinearity of a coherently coupled exciton-plasmon hybrid system under a strong control field with a weak probe field. The analytic formulas of exciton population and effective third-order optical susceptibility of the hybrid of a metal nanoparticle (MNP) and a semiconductor quantum dot (SQD) were deduced. The bistable exciton population and the induced bistable nonlinear absorption and refraction response were revealed. The bistability region can be tuned by adjusting the size of metal nanoparticle, interparticle distance and intensity of control field. Our results have perspective applications in optical information processing based on resonant coupling of exciton-plasmon.
A slow light effect in a hybrid nanocrystal complex composed of a semiconductor quantum dot (SQD) and a metal nanoparticle (MNP) is investigated theoretically. It is shown that a hole induced by coherent population oscillation appears at the absorption spectrum of the probe when an exciton and plasmon interact. Then a slow light effect may become possible. The numerical results further indicate that the slow light effect is greatly modified by the distance between the SQD and the MNP due to the coupling of the exciton and plasmon. For experimental conditions, the group velocity indexes with Gauss distribution and Lorenz distribution of the distance between the SQD and the MNP are evaluated. It is found that for small dispersion, almost the same values of the group velocity index can be obtained in these different distributions.