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Physical Review A

Effects of quantum coherence and interference in atoms near nanoparticles

Suman S. Dhayal, Yuri V. Rostovtsev

Published Apr 5, 2016• 15 citations
Publisher

Abstract

Optical properties of ensembles of realistic quantum emitters coupled to plasmonic systems are studied by using adequate models that can take into account full atomic geometry. In particular, the coherent effects such as forming ``dark states,'' optical pumping, coherent Raman scattering, and the stimulated Raman adiabatic passage (STIRAP) are revisited in the presence of metallic nanoparticles. It is shown that the dark states are still formed but they have more complicated structure, and the optical pumping and the STIRAP cannot be employed in the vicinity of plasmonic nanostructures. Also, there is a huge difference in the behavior of the local atomic polarization and the atomic polarization averaged over an ensemble of atoms homogeneously spread near nanoparticles. The average polarization is strictly related to the polarization induced by the external field, while the local polarization can be very different from the one induced by the external field. This is important for the excitation of single molecules, e.g., different components of scattering from single molecules can be used for their efficient detection.

DOI
10.1103/physreva.93.043405

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Optical properties of ensembles of realistic quantum emitters coupled to plasmonic systems are studied by using adequate models that can take into account full atomic geometry. In particular, the coherent effects such as forming ``dark states,'' optical pumping, coherent Raman scattering, and the stimulated Raman adiabatic passage (STIRAP) are revisited in the presence of metallic nanoparticles. It is shown that the dark states are still formed but they have more complicated structure, and the optical pumping and the STIRAP cannot be employed in the vicinity of plasmonic nanostructures. Also, there is a huge difference in the behavior of the local atomic polarization and the atomic polarization averaged over an ensemble of atoms homogeneously spread near nanoparticles. The average polarization is strictly related to the polarization induced by the external field, while the local polarization can be very different from the one induced by the external field. This is important for the excitation of single molecules, e.g., different components of scattering from single molecules can be used for their efficient detection.
The coherent effects such as forming “dark states,” optical pumping, and the stimulated Raman adiabatic passage (STIRAP) are studied in the presence of dielectric and/or metalic nanoparticles. It is shown that the “dark states” are still formed but they have more complicated atomic structure, the optical pumping and the STIRAP cannot be employed in the vicinity of plasmonic nanostructures. Also we show difference of the local atomic polarization and the atomic polarization averaged over ensemble of atoms homogeneously spread near nanoparticles.
We study the behavior of electric fields in and around dielectric and metal nanoparticles, and prepare the ground for their applications to a variety of systems viz. photovoltaics, imaging and detection techniques, and molecular spectroscopy. We exploit the property of nanoparticles being able to focus the radiation field into small regions and study some of the interesting nonlinear, and quantum coherence and interference phenomena near them. The traditional approach to study the nonlinear light-matter interactions involves the use of the slowly varying amplitude approximation (SVAA) as it simplifies the theoretical analysis. However, SVVA cannot be used for systems which are of the order of the wavelength of the light. We use the exact solutions of the Maxwell's equations to obtain the fields created due to metal and dielectric nanoparticles, and study nonlinear and quantum optical phenomena near these nanoparticles. We begin with the theoretical description of the electromagnetic fields created due to the nonlinear wavemixing process, namely, second-order nonlinearity in an nonlinear sphere. The phase-matching condition has been revisited in such particles and we found that it is not satisfied in the sphere. We have suggested a way to obtain optimal conditions for any type and size of material medium. We have also studied the modifications of the electromagnetic fields in a collection of nanoparticles due to strong near field nonlinear interactions using the generalized Mie theory for the case of many particles applicable in photovoltaics (PV). We also consider quantum coherence phenomena such as modification of dark states, stimulated Raman adiabatic passage (STIRAP), optical pumping in 444-level atoms near nanoparticles by using rotating wave approximation to describe the Hamiltonian of the atomic system. We also considered the behavior of atomic and the averaged atomic polarization in 777-level atoms near nanoparticles. This could be used as a prototype to study any n−n-n−level atomic system experimentally in the presence of ensembles of quantum emitters. In the last chapter, we suggested a variant of a pulse-shaping technique applicable in stimulated Raman spectroscopy (SRS) for detection of atoms and molecules in multiscattering media. We used discrete-dipole approximation to obtain the fields created by the nanoparticles.
This thesis is an attempt at studying quantum coherence effects coupled via plasmons. After introducing the quantum coherence in atomic systems in Chapter 1, we utilize it in Chapter 2 to demonstrate a new technique of detection of motion of single atoms or irons inside an optical cavity. By taking into account the interaction of coherences with surface plasmonic waves excited in metal nanoparticles, we provide a theoretical model along with experimental data in Chapter 3 to describe the modification of Raman spectra near metal nanoparticles. We show in chapter 4 that starting from two emitters, coupled via a plasmonic field, the symmetry breaking occurs, making detectable the simultaneous existence of the fast super-radiance and the slow sub-radiance emission of dye fluorescence near a plasmonic surface. In Chapter 5, we study the photon statistics of a group of emitters coupled via plasmons and by the use of quantum regression theorem, we provide a theoretical model to fully investigate the dependence of photon bunching and anti-bunching effects to the interaction between atoms, fields and surrounding mediums.
Optical properties of ensembles of three-level quantum emitters coupled to plasmonic systems are investigated employing a self-consistent model. It is shown that the stimulated Raman adiabatic passage (STIRAP) technique can be successfully adopted to control optical properties of hybrid materials with collective effects present and playing an important role in light-matter interactions. We consider a core-shell nanowire composed of a silver core and a shell of coupled quantum emitters and utilize a STIRAP scheme to control the scattering efficiency of such a system in a frequency and spatially dependent manner. After the STIRAP-induced population transfer to the final state takes place, the core-shell nanowire exhibits two sets of Rabi splittings with Fano line shapes, indicating strong interactions between two different atomic transitions driven by plasmon near-fields.
This review is devoted to the study of effects of quantum optics in nanostructures. The mechanisms by which the rates of radiative and nonradiative decay are modified are considered in the model of a two-level quantum emitter (QE) near a plasmonic nanoparticle (NP). The distributions of the intensity and polarization of the near field around an NP are analyzed, which substantially depend on the polarization of the external field and parameters of plasmon resonances of the NP. The effects of quantum optics in the system NP + QE plus external laser field are analyzed-modification of the resonance fluorescence spectrum of a QE in the near field, bunching/antibunching phenomena, quantum statistics of photons in the spectrum, formation of squeezed states of light, and quantum entangled states in these systems.
In this work, we present numerical results on the influence of a spherical metallic nanoparticle to the population transfer in a Λ-type quantum system under conditions of Stimulated Raman Adiabatic Passage (STIRAP). For the study of the system’s dynamics, we use the density matrix approach for the quantum system, where the parameters for the electric field amplitudes and the spontaneous decay rates have been calculated using ab initio electromagnetic calculations for the plasmonic nanoparticle. We present results for the evolution of the populations of the different levels of the quantum system as a function of different parameters, in the presence and the absence of the plasmonic nanoparticle. We find that the presence of the plasmonic nanoparticle and the polarization of the pump and Stokes fields with respect to the surface of the nanoparticle, affect the efficiency of the population transfer inside the three-level quantum system. For the right combination of the values of the modified spontaneous decay rates and the fields intensities, high efficiency population transfer is obtained in the quantum system near a plasmonic nanoparticle using STIRAP process.