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Ultrafast Energy Transfer Between Molecular Assemblies and Surface Plasmons in Hybrid Nano-Materials in the Strong Coupling Regime

Maxim Sukharev, Tamar Seideman, Robert J. Gordon, Adi Salomon, Yehiam Prior

Published Aug 22, 2013• 0 citations
OpenAlex

Abstract

The self-consistent model of coupled Maxwell-Liouville-von Neumann equations is used to scrutinize nonlinear dynamics of nano-materials comprised of interacting quantum emitters and plasmons. It is shown that ultra-short resonant laser pulses significantly modify optical properties of such hybrid systems. It is demonstrated that the energy transfer between interacting molecules and plasmons occurs on a femtosecond time scale. This energy transfer can be controlled with both materials parameters and laser radiation.

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Faraday Discussions•Oct 20, 2014•8 citations
The self-consistent model of coupled Maxwell-Liouville-von Neumann equations is used to scrutinize nonlinear dynamics of nano-materials comprised of interacting quantum emitters and plasmons. It is shown that ultra-short resonant laser pulses significantly modify optical properties of such hybrid systems. It is demonstrated that the energy transfer between interacting molecules and plasmons occurs on a femtosecond time scale. This energy transfer can be controlled with both materials parameters and laser radiation.
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.
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 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.
Nanoscale pulsed light is highly desirable in nano-integrated optics. In this paper, we obtained femtosecond pulses with THz repetition frequency via the coupling between quantum emitters (QEs) and plasmonic resonators. Our structure consists of a V\mathsf{V}V-groove (VG) plasmonic resonator and a nanowire embedded with two-level QEs. The influences of the incident light intensity and QE number density on the transmission response for this hybrid system are investigated through semiclassical theory and simulation. The results show that the transmission response can be modulated to the pulse form. And the repetition frequency and extinction ratio of the pulses can be controlled by the incident light intensity and QE number density. The reason is that the coupling causes the output power of nanowire to behave as an oscillating form, the oscillating output power in turn causes the field amplitude in the resonator to oscillate over time. A feedback system is formed between the plasmonic resonator and the QEs in the nanowire. This provides a method for generating narrow pulsed lasers with ultrahigh repetition frequencies in plasmonic systems using a continuous wave input, which has potential applications in generating optical clock signals at the nanoscale.
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 nanometers 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.
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.