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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Formation of dark states of atoms near metallic nanoparticles

Suman S. Dhayal, Yuri V. Rostovtsev

Published Mar 10, 2015• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.2086792

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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.
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.
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.
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.
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.
Abstract We investigate theoretically the population transfer process in a Λ-type three-level quantum system (QS) near a metallic nanosphere using the stimulated Raman adiabatic passage (STIRAP) technique. We combine density matrix quantum dynamical calculations with first-principle electromagnetic calculations, which quantify the influence of the plasmonic nanoparticle on the electric field of the pump and Stokes pulses in STIRAP as well as on the spontaneous emission rates within the Λ-type system. We study the population transfer process by varying the free-space spontaneous emission rate, the distance of the QS from the nanosphere, the polarization direction with respect to the nanoparticle surface and the relative strength of the pump and Stokes pulses used in STIRAP. We find that when the pump and Stokes fields have tangential and radial polarizations with respect to the nanosphere surface, the transfer efficiency is improved due to the increase of the decay rate of the excited state to the target state relatively to the decay to the initial state. The optimal population transfer is achieved for small interparticle distances, moderate free space spontaneous decay rate, large values of the pump Rabi frequency and small values of the Stokes Rabi frequency. When we exchange the polarization directions of the pump and Stokes fields we can still find a range of parameters where the population transfer remains efficient, but larger Stokes Rabi frequencies are necessary to overcome the increased decay rate from the excited state back to the initial state.
The preparation of an optically dense ensemble of three- level systems in dark states of the interaction with coherent radiation is discussed. It is shown that methods involving spontaneous emissions of photons such as Raman optical pumping fail to work beyond a critical density due to multiple scattering and trapping of these photons and the associated decay of the dark state(s). In optically thick media coherent-state preparation is only possible by entirely coherent means such as stimulated Raman adiabatic passage (STIRAP). It is shown that STIRAP is the underlying physical mechanism for electromagnetically induced transparency (EIT).