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The Journal of Physical Chemistry C

Control of Self-Kerr Nonlinearity in a Driven Coupled Semiconductor Quantum Dot–Metal Nanoparticle Structure

Spyridon G. Kosionis, Emmanuel Paspalakis

Published Mar 4, 2019• 42 citations
Publisher

Abstract

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.

DOI
10.1021/acs.jpcc.8b10817

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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.
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 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.
The emergence of hybrid nanostructures has paved a novel path for the development of nanotechnology and next-generation quantum devices.In this study, we report a remarkable enhancement of nonlinear diffraction achieved within a hybrid artificial molecule consisting of a semiconductor quantum dot (SQD) and a metal nanoparticle (MNP).Our findings reveal that the optical nonlinear properties of the hybrid system can be substantially enhanced due to the plasmon resonance of MNP.Specifically, reducing the interparticle distance and the SQD's size while increasing the MNP's size leads to a significant enhancement in the nonlinear phase modulation of the hybrid system.Meanwhile, the absorption spectra exhibit a redshift accompanied by linewidth broadening under the SQD-MNP coupling interaction controlled by geometric parameters, indicating plasmon-exciton energy transfer.On this basis, it is validated that the enhanced nonlinear phase modulation greatly improves the self-imaging visibility and the signal-to-noise ratio, and extends the near-field pattern over more Talbot lengths.We also demonstrate that the far-field diffraction efficiency is tunable via the coupling interaction between the artificial molecule and external fields, which is determined by the geometric structure, photon detuning, and Rabi frequency.For instance, the first-order diffraction efficiency can be increased from 39.58% to 55% if the geometric parameters of the hybrid system satisfy the threshold in non-resonance conditions.Such plasmon-enhanced optical lattices show potential for applications in all-optical modulators and all-optical switches operating at few-photon levels, and may also afford a novel perspective for the design and development of nanophotonics circuits and topological photonic devices.
Hybrid nanocomposites can provide a promising platform for integrated optics. Optical nonlinearity can significantly widen the range of applications of such structures. In the present paper, a theoretical investigation is carried out by solving the density matrix equations derived for a metal nanoparticles-graphene nanodisks-quantum dots hybrid system interacting with weak probe and strong control fields, in the steady state. We derive analytical expressions for linear and third-order nonlinear susceptibilities of the probe field. A giant self-Kerr nonlinear index of refraction is obtained in the optical region with relatively low light intensity. The optical absorption spectrum of the system demonstrates electromagnetically induced transparency and amplification without population inversion in the linear optical response arising from the negative real part of the polarizabilities for the plasmonic components at the energy of the localized surface plasmon resonance of the graphene nanodisks induced by the probe field. We find that the self-Kerr nonlinear optical properties of the system can be controlled by the geometrical features of the system, the size of metal nanoparticles and the strength of the control field. The controllable self-Kerr nonlinearities of hybrid nanocomposites can be employed in many interesting applications of modern integrated optics devices allowing for high nonlinearity with relatively low light intensity.
The optical nonlinearity of hybrid nanocrystal molecules composed of semiconductor and metal nanoparticles with a weak probe in a strong control field is investigated theoretically. Excitons in such a hybrid molecule demonstrate novel optical properties due to the coupling between excitons and plasmons. It is shown that Kerr nonlinear coefficients as functions of the detuning of the control field from the exciton frequency and the centre-to-centre distance between the two nanoparticles are greatly enhanced due to exciton–plasmon couplings.