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Journal of Luminescence

Phase-shifted response of plasmonic nanostructures: Implications to luminescence upconversion

Khachatur Nerkararyan, Torgom S. Yezekyan, Sergey I. Bozhevolnyi

Published Jul 27, 2017• 4 citations
Publisher

Abstract

We analyze the dynamics of a quantum dipole emitter (QDE) illuminated by a resonant electromagnetic field and placed close to a metal nanostructure, whose response to the incident field is phase shifted by 3π/2 (-π/2). It is found that, due to the phase shift in a field scattered by the nanostructure (and acting on the QDE along with the incident field), QDE dynamics is characterized by a fast QDE transition to the excited state followed by relaxation to a stable superposition (of the excited and ground states) with a close to 1 probability of the QDE to be found in the excited state. We further argue that this effect can advantageously be used for luminescence upconversion enhancement when being realized for a lower excited state in the energy transfer upconversion process since, by largely eliminating the radiative relaxation channel, the probability of excitation transfer will be increased.

DOI
10.1016/j.jlumin.2017.07.047

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We analyze the dynamics of a quantum dipole emitter (QDE) illuminated by a resonant electromagnetic field and placed close to a metal nanostructure, whose response to the incident field is phase shifted by 3π/2 (-π/2). It is found that, due to the phase shift in a field scattered by the nanostructure (and acting on the QDE along with the incident field), QDE dynamics is characterized by a fast QDE transition to the excited state followed by relaxation to a stable superposition (of the excited and ground states) with a close to 1 probability of the QDE to be found in the excited state. We further argue that this effect can advantageously be used for luminescence upconversion enhancement when being realized for a lower excited state in the energy transfer upconversion process since, by largely eliminating the radiative relaxation channel, the probability of excitation transfer will be increased.
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.
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 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.
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 develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nm from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
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.