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arXiv:1311.5476 · Optics Letters

Relaxation dynamics of a quantum emitter resonantly coupled to a metal nanoparticle

Khachatur Nerkararyan, Sergey I. Bozhevolnyi

Published Mar 11, 2014• 22 citations
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Abstract

The presence of a metal nanoparticle (MNP) near a quantum dipole emitter, when a localized surface plasmon mode is excited via the resonant coupling with an excited quantum dipole, dramatically changes the relaxation dynamics: an exponential decay changes to step-like behavior. The main physical consequence of this relaxation process is that the emission, being largely determined by the MNP, comes out with a substantial delay. A large number of system parameters in our analytical description opens new possibilities for controlling quantum emitter dynamics.

DOI
10.1364/ol.39.001617

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The presence of a metal nanoparticle (MNP) near a quantum dipole emitter, when a localized surface plasmon mode is excited via the resonant coupling with an excited quantum dipole, dramatically changes the relaxation dynamics: an exponential decay changes to step-like behavior. The main physical consequence of this relaxation process is that the emission, being largely determined by the MNP, comes out with a substantial delay. A large number of system parameters in our analytical description opens new possibilities for controlling quantum emitter dynamics.
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.
We investigate 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. 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. It is also shown that energy dissipation in the QDE-MNP system is relatively weak with the probability of the photon emission being about 0.75, a number which, rather surprisingly, does not explicitly depend on the metal absorption characteristics. The degree of entanglement measured by the concurrency takes the maximum value, while the distances between the QDEs and metal ball approximately are equal.
We investigate relaxation dynamics in the system of two identical quantum dipole emitters (QDEs) located near a metal nanoparticle (MNP) exhibiting a dipolar localized surface plasmon (LSP) resonance at the frequency of the QDE radiative transition. Considering one QDE to be brought into an optically active excited state and weakly coupled to the resonant LSP, we show that a stable superposition state of two QDEs is formed during the transition time, which is much shorter than the QDE spontaneous decay time and determined by the efficiency of resonant interaction between the QDEs and induced LSP. It is elucidated that the superposition state is established as a result of redistribution of the energy of the initially excited QDE so that the corresponding steady-state QDE fields induced at the MNP site cancel each other. The degree of steady-state entanglement characterized by the concurrence is found dependent only on the ratio of distances between the QDEs and the MNP, reaching its maximum value of $\ensuremath{\sim}0.65$, when the separation between the MNP and the initially excited QDE is larger by $\ensuremath{\sim}20%$ than the distance from the other QDE to the MNP.
We investigate excitation dynamics in the system of a quantum dipole emitter (QDE) coupled to a located nearby metal nanoparticle (MNP), which exhibits a dipolar localized surface plasmon (LSP) resonance at the frequency of the QDE radiative transition, in the presence of a strong external resonant electromagnetic field. Considering the QDE-field interactions in the regime of strong QDE-field coupling, we show that the feedback provided by the MNP on the QDE (due to the LSP excitation with the field generated by the dipole moment of the QDE transition) influences significantly the coherent process of Rabi oscillations, resulting in the occurrence of additional satellite frequencies in the radiation spectrum scattered by the QDE-MNP configuration. The relative ratio of high harmonics depends strongly on the QDE-MNP separation, an important characteristic feature that can be used for observing this effect and can be exploited, for example, for controlling distances at the nanoscale.
The relaxation dynamics of a quantum dipole emitter coupled to a metal nanostructure in the presence of an external resonant pump field is studied. It was found that in the mode of weak pumping, the phase of the response from a metallic nanostructure plays a key role in the dynamics of the quantum dipole emitter and allows one to control the fluorescence process. It is shown that when the phase shift is set close to π/2, the quantum emitter makes a quick transition into the ground state, then slowly passes into a superposition state with a small probability to remain in an excited state. Meanwhile, in the case of phase shift values close to 3π/2, the system relaxes into a stationary superposition state where the probability to be in the excited state is close to unity. It was established that the dynamics of the system also depends on the intensity of the external field and with the amplification of the latter, the system enters into the mode of the asymmetric Rabi oscillations.
In this work phenomenon of resonant transfer of the excited energy between quantum dipole emitters (QDE) by the localized plasmon polaritons (LPP) is investigated. In system the molecules or semiconductor quantum dots act as QDEs and the nanometer size metal particles (MNP) care LPPs. The dependence of the frequency of Rabi oscillations on system parameters (the distance between MNP and QDE, the radius of MNP and dielectric permittivity of the surrounding medium) was determined. Conditions when the period of Rabi oscillations is considerably shorter than system relaxation time were defined.