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International Online Conference on Nanomaterials (IOCN)

Four-Wave Mixing in Asymmetric Double Quantum Dot Molecule–Metal Nanoparticle Assemblies

Spyridon G. Kosionis, Emmanuel Paspalakis

Published Nov 11, 2020• 2 citations
Publisher

Abstract

In this study, the four-wave mixing (FWM) spectrum of a strongly pumped hybrid structure is theoretically examined. The hybrid structure consists of an asymmetric double semiconductor quantum dot (SQD) molecule and a spherical metal nanoparticle (MNP), which are coupled together via long-range Coulomb interaction. Having as a starting point the Hamiltonian of the system, in the dipole and the rotating-wave approximations, we derive a set of nonlinear density matrix equations, which are numerically solved, in the steady-state limit, and then the FWM coefficient is calculated within a range of values of the pump–probe field detuning. The spectral response of the FWM coefficient is investigated, for different values of the pump-field detuning, the electron-tunneling rate, and the energy gap between the upper states in the energy-level scheme of the double SQD molecule, while the interparticle distance between the two components of the structure is modified.

DOI
10.3390/iocn2020-07843

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In this study, the four-wave mixing (FWM) spectrum of a strongly pumped hybrid structure is theoretically examined. The hybrid structure consists of an asymmetric double semiconductor quantum dot (SQD) molecule and a spherical metal nanoparticle (MNP), which are coupled together via long-range Coulomb interaction. Having as a starting point the Hamiltonian of the system, in the dipole and the rotating-wave approximations, we derive a set of nonlinear density matrix equations, which are numerically solved, in the steady-state limit, and then the FWM coefficient is calculated within a range of values of the pump–probe field detuning. The spectral response of the FWM coefficient is investigated, for different values of the pump-field detuning, the electron-tunneling rate, and the energy gap between the upper states in the energy-level scheme of the double SQD molecule, while the interparticle distance between the two components of the structure is modified.
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 (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.
We investigate how the four-wave mixing (FWM) spectrum of a hybrid nanostructure, comprising a semiconductor quantum dot coupled to an ellipsoidal metal nanoparticle and interacting with a weak probe and strong pump electromagnetic field, depends on various parameters, including interparticle distance, the length and orientation of the polar semiaxis of the ellipsoidal nanoparticle, the polarization direction of the fields, and the detuning of the pump field. We present a general analytical steady-state solution for the density matrix elements and use this solution to define the effective Rabi frequency and detuning parameters, which are incorporated into a dressed-state framework. This approach reveals the impact of these physical parameters on the number, position, and width of resonances in the FWM spectrum, offering insights into their underlying mechanisms.
We investigate theoretically four-wave mixing (FWM) response and optical bistability (OB) in a hybrid nanosystem composed of a metal nanoparticle (MNP) and a semiconductor quantum dot (SQD) coupled to a nanomechanical resonator (NR). It is shown that the FWM signal is enhanced by more than three orders of magnitude as compared to that of the system without exciton-phonon interaction, and the FWM signal can also be suppressed significantly and broadened due to the exciton-plasmon interaction. As the MNP couples strongly with the SQD, the bistable FWM response can be achieved by adjusting the SQD-MNP distance and the pumping intensity. For a given pumping constant and a fixed SQD-MNP distance, the enhanced exciton-phonon interaction can promote the occurrence of bistability. Our findings not only present a feasible way to detect the spacing between two nanoparticles, but also hold promise for developing quantum switches and nanoscale rulers.
We investigate the optical properties appearing in a nanostructure that is composed of an asymmetric double semiconductor quantum dot (SQD) molecule and a metal nanoparticle (MNP). The profile of the total linear absorption spectrum is proportional to the SQD contribution, while the MNP contribution is important. The profile of the doublet of resonances detected on the total linear absorption spectrum creates a transparency window. The doublet is asymmetric for small SQD-MNP distances and has a narrow peak and a wide peak. The width of the transparency window is increased, either with the enhancement of the rate at which the electron tunneling effect takes place within the double SQD molecule or with the decrease of the distance that separates the SQD molecule from the center of the MNP. The steep slope detected on the linear dispersion spectrum for frequencies laying within the transparency window owes its presence to the tunneling induced transparency and leads to slow light production. The corresponding value of the slow down factor is maximized for low values of the electron tunneling rate as well as for low center-to-center distances between the components of the hybrid nanostructure.
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.