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Journal of the Optical Society of America B

Effect of dipole–dipole interactions on the one-photon and two-photon photoluminescence in an ensemble of quantum dots doped in a polymer matrix

Patrick D. Persaud, Mahi R. Singh

Published Oct 8, 2020• 15 citations
Publisher

Abstract

We have developed a theory for the one-photon and two-photon fluorescence of a nanohybrid composite comprised of an ensemble of quantum dots encased in a matrix of polymer. The quantum dots are comprised of four-level quantum emitters encased within a coating of dielectric material. The fluorescence of the quantum dot system is calculated using the master equation method where dipole–dipole interaction (DDI) coupling is present. The application of a probe field to the nanohybrid composite material in conjunction with the DDI between the quantum dots generates an enhancement of both the single-photon and double-photon fluorescence, and in certain conditions causes spectrum splitting. With a strong DDI field, the two-photon emission spectrum experiences slight quenching and shifts from one peak to two peaks. The dressed states are a result of strong coupling effects between the DDI field and the quantum dots. We generated an analytical expression for the fluorescence spectrum and intensity, and quantitatively compared it to experimental data in which ZnSe quantum dots were embedded within a P3HT polymer film, with our theory strongly correlating with the experiment. We also quantitatively compared our theory with experimental data that demonstrated the single-photon emission spectrum of colloidal quantum dots comprised of a CdZnS/ZnS gradient structure in varying probe field strengths. We found that our theory predicted the spectrum peak splitting that the experiment produced.

DOI
10.1364/josab.404007

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We have developed a theory for the one-photon and two-photon fluorescence of a nanohybrid composite comprised of an ensemble of quantum dots encased in a matrix of polymer. The quantum dots are comprised of four-level quantum emitters encased within a coating of dielectric material. The fluorescence of the quantum dot system is calculated using the master equation method where dipole–dipole interaction (DDI) coupling is present. The application of a probe field to the nanohybrid composite material in conjunction with the DDI between the quantum dots generates an enhancement of both the single-photon and double-photon fluorescence, and in certain conditions causes spectrum splitting. With a strong DDI field, the two-photon emission spectrum experiences slight quenching and shifts from one peak to two peaks. The dressed states are a result of strong coupling effects between the DDI field and the quantum dots. We generated an analytical expression for the fluorescence spectrum and intensity, and quantitatively compared it to experimental data in which ZnSe quantum dots were embedded within a P3HT polymer film, with our theory strongly correlating with the experiment. We also quantitatively compared our theory with experimental data that demonstrated the single-photon emission spectrum of colloidal quantum dots comprised of a CdZnS/ZnS gradient structure in varying probe field strengths. We found that our theory predicted the spectrum peak splitting that the experiment produced.
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 study the coupling between quantum dots through the dipole–dipole interaction in photonic nanofibers manufactured by embedding a dielectric material into a photonic crystal. The embedded dielectric material is doped with an ensemble of three-level quantum dots. A probe field is applied to monitor the absorption, and a control field is applied to induce dipole moments in quantum dots. Dipoles are induced in quantum dots due to the external fields, and they interact with each other via the dipole–dipole interaction. Quantum dots also interact with the nanofiber through the electron–bound photon interaction. The absorption coefficient has been calculated using the density matrix method, and the dipole–dipole interaction has been evaluated in the mean field approximation. It is found that the absorption spectrum splits from one peak to two peaks by the dipole–dipole interaction. The splitting of peaks can be controlled by either the resonance energy of quantum dots or bound photon states of the nanofiber.
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.
The effect of the dipole-dipole interaction (DDI) on absorption processes has been investigated in photonic nanowires. They are manufactured by embedding a photonic crystal into another crystal. The embedded crystal is doped with an ensemble of three-level quantum dots. A probe field is applied to monitor the absorption coefficient. A control field is applied to induce dipole moments in quantum dots. Owing to these fields dipoles are induced in quantum dots, and they interact with each other via the DDI. Quantum dots also interact with bound photon states of the nanowire via the electron-bound photon interaction. It is found that the system can be switched from a transparent state to an absorbing state through the DDI. The switching mechanism can be controlled by changing the location of a resonant energy in the quantum dots.
Quantum optics provides a fundamental framework for understanding the interaction between light and matter at the quantum level. Recently, it has been shown that under incoherent pumping, the resonance fluorescence spectrum dramatically changes. Engineering the resonance fluorescence spectrum paves the way towards solid-state-based single-photon sources. In this paper, we start by reviewing and reproducing some of the results concerning the resonance fluorescence spectrum, single-photon sources, dressed-state lasers, and luminescence spectrum of a quantum dot in a microcavity. Photon correlations in quantum optical systems and spectral properties of radiation emitted by atomic and semiconductor systems interacting with external fields are investigated. The well known Mollow triplet structure of the emission spectrum is discussed, together with the role of dressed states in explaining the origin of the three spectral peaks. Furthermore, the luminescence spectra of quantum emitters coupled to microcavities are reviewed. The numerical results presented here contribute to the theoretical understanding of resonance fluorescence, photon correlations, and engineered emission in quantum optical systems. These studies highlight the rich physical properties arising from light matter interaction at the quantum level and demonstrate their relevance for emerging quantum technologies.
Abstract The dipole–dipole interaction (DDI) has been studied in photonic quantum wells are simulated from two photonic crystals say A and B. An ensemble of nanoparticles is doped within the quantum well layer. Nanoparticles are interacting with each other via DDI. The absorption spectrum has been calculated by using the time dependent Schrodinger equation method. A probe field is applied to measure the absorption spectrum. Numerical simulations for the absorption coefficient have been performed. It has been found that in the absence of DDI the spectrum has two peaks and a minimum at zero detuning. However, in the presence of the large DDI coupling both peaks disappear and a large minimum appears. This means that the positions and heights of peaks can be changed due to DDI interaction. This study can be used to make new types of optical devices. (© 2009 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)