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arXiv:1206.5439 · Physical Review A

Stimulated Raman adiabatic passage as a route to achieving optical control in plasmonics

Maxim Sukharev, Svetlana Malinovskaya

Published Oct 4, 2012• 28 citations
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Abstract

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.

DOI
10.1103/physreva.86.043406

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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.
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.
Optical properties of ensembles of coupled three-level quantum emitters are investigated in linear and non-linear regimes. The model of the Maxwell–Liouville von Neumann equations is implemented to explore the reflection, transmission, and absorption of a thin layer of atom-like emitters at low and high densities. The stimulated Raman adiabatic passage is analysed in systems of coupled quantum emitters of various densities. It is shown that coupling via local electromagnetic fields shifts the energy levels and modifies propagating fields leading to a mixed final population distribution and appearance of new absorption resonances. Strong femtosecond pulses induce population inversion in emitters leading to optical gain.
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 coupled three-level quantum emitters are investigated in linear and non-linear regimes. The model of the Maxwell–Liouville von Neumann equations is implemented to explore the reflection, transmission, and absorption of a thin layer of atom-like emitters at low and high densities. The stimulated Raman adiabatic passage is analysed in systems of coupled quantum emitters of various densities. It is shown that coupling via local electromagnetic fields shifts the energy levels and modifies propagating fields leading to a mixed final population distribution and appearance of new absorption resonances. Strong femtosecond pulses induce population inversion in emitters leading to optical gain.
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.
We investigate collective chirped stimulated Raman adiabatic passage (STIRAP) in a pair of identical three-level atoms using a symmetric six-state model. Numerical simulations reveal a pronounced oscillatory dependence of the population transfer to the doubly excited Rydberg state on the peak Rabi frequency, indicating dynamics beyond the conventional single-dark-state description of STIRAP. To identify the underlying mechanism, we develop a dressed-manifold description based on gauge-invariant projections onto nearly degenerate instantaneous dressed manifolds. The analysis demonstrates that the wavefunction remains predominantly confined to a two-dimensional dark manifold while becoming transiently coupled to a neighboring bright manifold during the pulse-overlap interval. We further show that in the dressed-manifold representation, the Rydberg-Rydberg interaction modifies the collective resonance structure while preserving the dark-bright manifold dynamics responsible for the oscillatory transfer; an appropriately chosen frequency chirp compensates the interaction-induced detuning and restores efficient population transfer. This dressed-manifold picture provides a consistent interpretation of oscillatory collective transfer and establishes a framework for controlling adiabatic dynamics in interacting multilevel systems by linearly chirped STIRAP, opening a route toward manifold-based control of Rydberg-mediated quantum gates, correlated-state preparation, and other coherent operations in interacting atomic systems.