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

Transient plasmon-like modes in multi-level quantum emitter systems

Martin J. Gentile, William L. Barnes

Published Sep 10, 2014• 0 citations
Publisher

Abstract

We model a nanoparticle of organic dye molecules as an ensemble of multi-level quantum systems in order to determine the conditions necessary to yield temporal optical field enhancement for different probe energies. By utilizing a time-dependent density-matrix approach and by examination of the role played by both radiative and non-radiative decay processes between energy levels, we explore how optical pump and probe fields may be used to control the permittivity of the nanoparticle as a function of time. When an appropriate value of the permittivity occurs, a plasmon-like mode will be produced. In this work, we investigate systems in which these plasmon-like modes can be generated at probe energies detuned from the atomic transitions and sustained for timescales dependent on the lifetime of a meta-stable level in our system. Our results suggest that these plasmon-like modes may generate temporal optical field enhancement and that such nanostructures open a new realm in nanophotonics in which transient behaviour can lead to phenomena that cannot be attained in the steady-state regime.

DOI
10.1117/12.2061004

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We model a nanoparticle of organic dye molecules as an ensemble of multi-level quantum systems in order to determine the conditions necessary to yield temporal optical field enhancement for different probe energies. By utilizing a time-dependent density-matrix approach and by examination of the role played by both radiative and non-radiative decay processes between energy levels, we explore how optical pump and probe fields may be used to control the permittivity of the nanoparticle as a function of time. When an appropriate value of the permittivity occurs, a plasmon-like mode will be produced. In this work, we investigate systems in which these plasmon-like modes can be generated at probe energies detuned from the atomic transitions and sustained for timescales dependent on the lifetime of a meta-stable level in our system. Our results suggest that these plasmon-like modes may generate temporal optical field enhancement and that such nanostructures open a new realm in nanophotonics in which transient behaviour can lead to phenomena that cannot be attained in the steady-state regime.
Abstract Quantum coherence and interference offer novel pathways to control light–matter interaction at the atomic scale, with enticing prospects in both fundamental and applied science. Here, we demonstrate coherent control over transient excitation of localized surface plasmon modes of a silver nanosphere adjacent to a quantum coherence medium composed of three-level quantum emitters, using a theoretical approach. We show that quantum interference enables more than two orders of magnitude enhancement in the surface plasmon field generated when the quantum emitters are driven coherently, in comparison to incoherent pumping. Furthermore, under optimal conditions, intense surface plasmon lasing can be induced without population inversion on the spasing transition. Our results open up the possibility of overcoming dissipative losses in plasmonic modes in the transient regime when steady-state population inversion is difficult to achieve due to fast relaxation rates and impractical pumping requirements.
We investigate the relaxation dynamics of a quantum dipole emitter (QDE), e.g., a molecule or quantum dot, located near a metal nanoparticle (MNP) exhibiting a dipolar localized surface plasmon (LSP) resonance at the frequency of the QDE radiative transition. A generic three-level QDE, which is pumped with an external laser pulse and thereby brought into an optically active excited state, is considered to be weakly coupled to the resonant LSP described by a coherent state. It is shown that, under the condition of the QDE-MNP characteristic relaxation time being much shorter than that of the QDE in free space but much longer than the LSP lifetime, the QDE relaxation dynamics can be described analytically and feature, in general, non-exponential decay with complicated transient behaviour. The main physical consequence of this relaxation process is that the emission, being largely determined by the MNP, comes out with a substantial delay. It is also shown that energy dissipation in the QDE-MNP system is relatively weak with the probability of the photon emission being ∼0.75, a number which, rather surprisingly, does not explicitly depend on the metal absorption characteristics. A large number of QDE-MNP system parameters in our analytical description open new possibilities for controlling quantum emitter dynamics.
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.
Hybridization of quantum emitters and plasmonic nanostructures has attracted much attention over the last years, due to their potential use as plasmon-based nanolasersor to achieve long-range quantum bit entanglement. Recent theoretical studies suggest that the plasmonic field can induce efficient cross-talking between emitters and lead to the formation of collective superradiant states. In this thesis, we developed a theoretical modelable to analyse collective effects in large ensemble of dipoles coupled by an electromagnetic nanoresonator. We experimentally investigated the plasmon-mediated superradiance of organic emitters grafted at a well-controlled distance from a metal nanosphere at room temperature. We report on the measured decay rates of these hybrid structures at the ensemble and single object levels. We find that the decay rate increases i) with the number ofemitters and ii) as the spacing between the emitters and the metal core decreases, a direct and clear evidence of plasmonic superradiance. This trend was observed for two types of hybrid structures, differing both by the size of the metal core and the type of organic dye used as emitter. The observation of plasmonic superradiance at room temperature opens questions about the robustness of these collective states against decoherence mechanisms.This robustness is of major interest for potential applications of quantum systems at room temperature.
We analyze the two-time intensity correlation function of the fluorescent field emitted by a three-level V-type quantum emitter located in the vicinity of a two-dimensional periodic plasmonic nanostructure. Due to the interaction of the quantum emitter with an electromagnetic field, the ground state population is excited to the upper levels, presenting decay due to spontaneous emission. The distinctive characteristic of this system is that the decay rates for a quantum emitter with dipole orientation perpendicular and normal to the surface of the nanostructure array exhibit large differences which vary with the distance between the quantum emitter and the two-dimensional nanoparticle array. This leads to simulation of quantum interference effects in spontaneous emission. By studying the dependence of the two-time intensity correlation function on specific physical parameters of the hybrid structure, including the intensity of the applied field, the detuning from resonance, the distance between the quantum emitter and the plasmonic nanostructure, as well as the spacing between the upper levels, we demonstrate a strong modification of the two-time intensity correlation functions. We also identify the conditions under which the two-time intensity correlation function is maximized, an effect which is associated to the bunching to antibunching transition of the emitted photons.
We have studied the electromagnetically induced transparency for a two level ensemble interacting with two orthogonal optical modes. We have made a approach for a multimode silicon waveguide coupled to a plasmonic resonator array. We have shown that a simple periodic ensemble of resonant metal nanoparticles within a dielectric waveguide supported a transparent waveguide plasmon polariton mode for guided slow light propagation. Such systems inhert the strongly dispersive properties of the nanoparticles embedded in the waveguide but do not succumb to the associated absorptive losses by utilizing the system’s transparency Light propagation through the system provided extremely strong dispersion from the resonators, but suffers very low propagation loss by exploiting the system’s transparency. Dispersion is controllable by tuning the coupling strength of localized plasmon and waveguide modes. We have found that atomic electromagnetically induced transparency occurred for a non zero pump field allowing mutual coupling of all states and induced destructive quantum interference of the probe field’s absorption via the transition. The obtained results were found in good agreement with previously obtained results.