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Journal of the Optical Society of America B

Nonlinear energy transfer in quantum dot and metallic nanorod nanocomposites

Mahi R. Singh, Chris Racknor

Published Sep 29, 2015• 24 citations
Publisher

Abstract

We have investigated the nonlinear energy transfer in a quantum dot (QD) and metallic nanorod (MNR) nanocomposite. An intense probe laser field is applied to monitor two-photon energy transfer from the QD to the MNR and a control laser field is applied to control the energy transfer rate. Induced dipoles are created in the QD and MNR and these dipoles are interacting with each other. Surface plasmon resonances (SPRs) are also created in the MNR due to a coupling of charge fluctuations and external laser fields. Therefore, there is a dipole–dipole interaction between excitons in the QD and SPRs in the MNR. Due to this interaction, the two-photon energy is transferred from the QD to the MNR. Using the density matrix method, the energy transfer rate between the components of the system is evaluated. It is found that the energy transfer rate has one peak due to the transfer of the two-photon energy from the QD to the MNR when the control field is absent. When the control field is applied, this peak disappears. This means no energy transfer between two components of the nanosystems. However, two new peaks appear in the energy transfer rate at two different energies. It is also found that by varying the intensity of the probe field, one can also control the energy transfer from the QD to the MNR. These are interesting findings of the paper and they can be used to fabricate nanosensors, nanoswitches, and energy transfer devices.

DOI
10.1364/josab.32.002216

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We have investigated the nonlinear energy transfer in a quantum dot (QD) and metallic nanorod (MNR) nanocomposite. An intense probe laser field is applied to monitor two-photon energy transfer from the QD to the MNR and a control laser field is applied to control the energy transfer rate. Induced dipoles are created in the QD and MNR and these dipoles are interacting with each other. Surface plasmon resonances (SPRs) are also created in the MNR due to a coupling of charge fluctuations and external laser fields. Therefore, there is a dipole–dipole interaction between excitons in the QD and SPRs in the MNR. Due to this interaction, the two-photon energy is transferred from the QD to the MNR. Using the density matrix method, the energy transfer rate between the components of the system is evaluated. It is found that the energy transfer rate has one peak due to the transfer of the two-photon energy from the QD to the MNR when the control field is absent. When the control field is applied, this peak disappears. This means no energy transfer between two components of the nanosystems. However, two new peaks appear in the energy transfer rate at two different energies. It is also found that by varying the intensity of the probe field, one can also control the energy transfer from the QD to the MNR. These are interesting findings of the paper and they can be used to fabricate nanosensors, nanoswitches, and energy transfer devices.
We have studied quantum coherence and interference phenomena in a quantum dot (QD)-metallic nanorod (MNR) hybrid system. Probe and control laser fields are applied to the hybrid system. Induced dipole moments are created in the QD and the MNR, and they interact with each other via the dipole-dipole interaction. Using the density matrix method, it was found that the power spectrum of MNR has two transparent, states and they can be switched to one transparent state by the control field. Ultrafast switching and sensing nanodevices could be produced using this model.
We have developed a theory for the two-photon fluorescence in nanohybrids made of an ensemble of metallic nanorod shells and an ensemble of quantum emitters. A metallic nanorod shell is made of a metallic rod and dielectric shell. We consider that the quantum emitters are four-level quantum systems. When a probe laser light falls on the metallic nanorod shells, the surface plasmon polariton electric field is produced at the interface between the metallic nanorod and dielectric shell. This electric field, along with the probe field, induces dipoles in the quantum emitters and nanorod shells. These dipoles interact with each other via the dipole–dipole interaction. The two-photon fluorescence has been calculated by using the quantum density matrix method in the presence of the dipole–dipole interaction (coupling). Analytical expressions of the two-photon fluorescence have been derived in the presence of the dipole–dipole interaction. We showed that that the two-photon process is made of two terms. The first term is the two-photon process due to the two probe field photons. On other the hand, the second term is made of one DDI field photon and one probe field photon. It is found that the surface plasmon polariton resonance energy is not resonant with the exciton energy, the two-photon fluorescence spectrum splits from one peak to three peaks. The splitting in the spectrum is due to the presence of the dressed states created in the system due to the strong dipole–dipole interaction. We also compared our theory with the experimental data of the metallic nanohybrid system made of metallic nanorod shells and quantum emitters (T790 molecules) and found a good agreement between the theory and the experiments.
We have studied energy absorption rate in a quantum dot-metallic nanosphere system embedded on a dielectric substrate. We applied a control field to induce dipole moments in the quantum dot and the metal nanosphere, and monitored the energy absorption using a probe field. These external fields induce dipole moments in the metal nanosphere and the quantum dot, and these two structures interact with one another via the dipole-dipole interaction. The density matrix method was used to evaluate the absorption, indicating that it can be shifted by moving the metal nanosphere close to the quantum dot. Also, absorption efficiency can either be quenched or enhanced by the addition of a metal nanosphere. This hybrid system can be used to create ultrafast switching and sensing nanodevices.
A theory of a switching and sensing mechanisms using the Kerr nonlinearity has been developed for nanohybrids made of an ensemble of three-level quantum emitters and metallic nanoshells. We have calculated the surface plasmon polaritons at interface between the metallic core and dielectric shell of the metallic nanoshell. The Kerr nonlinearity has been calculated by using the quantum density matrix method in the dipole–dipole coupling between quantum emitters. We showed that the switching and sensing mechanisms due to the Kerr nonlinearity are made of four contributions. The first contribution is due to three probe photons and the second one is due to one polariton and two probe photons. On other hand, the third contribution is due to the two polaritons and one probe photon, and the fourth one is due to three polaritons. The enhancement in the Kerr nonlinearity is found, and it is due to second, third, and fourth contributions. This prediction can be used to fabricate all optical Kerr nanosensors. It is also shown that two peaks (ON) in the Kerr coefficient can be switched to four peaks (OFF) due to the strong dipole–dipole coupling. We have also predicted that the Kerr coefficient can be switched from the positive value (ON) to the negative value (OFF) by changing the dipole–dipole coupling. We found that the minimum of the Kerr coefficient changes sign from positive (ON) to negative (OFF) as the dipole–dipole coupling strength increases. The splitting in the Kerr spectrum is due to the presence of the dressed states created in the nanohybrid due the dipole–dipole interaction. These predictions can be used to fabricate all optical Kerr nanoswitches.
In this review article, we discuss the many-body interactions in plasmonic nanohybrids made of an ensemble of quantum emitters and metallic nanoparticles. A theory of the linear and nonlinear optical emission intensity was developed by using the many-body quantum mechanical density matrix method. The ensemble of quantum emitters and metallic nanoparticles interact with each other via the dipole-dipole interaction. Surfaces plasmon polaritons are located near to the surface of the metallic nanoparticles. We showed that the nonlinear Kerr intensity enhances due to the weak dipole-dipole coupling limits. On the other hand, in the strong dipole-dipole coupling limit, the single peak in the Kerr intensity splits into two peaks. The splitting of the Kerr spectrum is due to the creation of dressed states in the plasmonic nanohybrids within the strong dipole-dipole interaction. Further, we found that the Kerr nonlinearity is also enhanced due to the interaction between the surface plasmon polaritons and excitons of the quantum emitters. Next, we predicted the spontaneous decay rates are enhanced due to the dipole-dipole coupling. The enhancement of the Kerr intensity due to the surface plasmon polaritons can be used to fabricate nanosensors. The splitting of one peak (ON) two peaks (OFF) can be used to fabricate the nanoswitches for nanotechnology and nanomedical applications.
Abstract A theory of the two-photon florescence for a metallic nanoshell in the presence of quantum emitters has been developed. The metallic nanoshell is made of a metallic nanosphere as a core and a dielectric material as a shell. An ensemble of quantum emitters is deposited on the surface of the dielectric shell. A probe field is applied to study the two-photon process in the metallic nanoshell. Surface plasmon polaritons are created at the interface between the core and shell due to coupling between probe photons and surface plasmons present at the surface of the metallic nanosphere. The intensity of the surface plasmon polariton field is huge when the probe photon energy is in resonance with the polariton resonance energy. Induced electric dipoles are created in each quantum emitter due to the surface plasmon polariton field and the probe field. Dipoles in quantum emitters interact with each other via the dipole-dipole interaction. The dipole-dipole interaction is calculated using the many-body theory and mean field approximation. It is found that the dipole-dipole interaction has new term which is induced by the surface plasmon polariton field. An analytical expression of the two-photon florescence is derived in the presence the dipole-dipole interaction. Our theory predicts that the intensity of the two-photon florescence is enhanced in the presence of quantum emitters relative to the florescence of the metallic nanoshell in isolation. Physics behind the enhancement is the presence of the dipole-dipole interaction between the ensemble of quantum emitters. It is also found that as the concentration of quantum emitters increases, the dipole-dipole field also increases. This in turn, increases the two-photon florescence as function of the concentration. Finally, we have compared our theory with experiments of a metallic nanoshell which is made for Au nanosphere core and the SiO 2 shell. The metallic nanoshell is surrounded by various concentrations of Cadmium-Selenium quantum dots as quantum emitters. A good agreement between theory and experiment is found.