Cooperative Energy Transfer Controls the Spontaneous Emission Rate Beyond Field Enhancement Limits

Abstract

Quantum emitters located in proximity to a metal nanostructure individually transfer their energy via near-field excitation of surface plasmons. The energy transfer process increases the spontaneous emission (SE) rate due to plasmon-enhanced local field. Here, we demonstrate significant acceleration of quantum emitter SE rate in a plasmonic nano-cavity due to cooperative energy transfer (CET) from plasmon-correlated emitters. Using an integrated plasmonic nano-cavity, we realize up to six-fold enhancement in the emission rate of emitters coupled to the same nano-cavity on top of the plasmonic enhancement of the local density of states. The radiated power spectrum retains the plasmon resonance central frequency and lineshape, with the peak amplitude proportional to the number of excited emitters indicating that the observed cooperative SE is distinct from super-radiance. Plasmon-assisted CET offers unprecedented control over the SE rate and allows to

Plasmon-Field-Induced Metastable States in the Wetting Layer: Detected by the Fluorescence Decay Time of InAs/GaAs Single Quantum Dots

“…In general, light-matter interaction is realizable in the vicinity of the metal nanoparticles. It includes enhancing or quenching fluorescence radiation and a cooperative emission of light by the ensemble of emitter dipoles near metal nanoparticles [9,[15][16][17][18]. Considering a system of an emitter nearby metal particles, if small particles have a radius of , the total electric field at the emitter site is the sum of the emitter's own field and dipole field of particles , [10,19].…”

“…Such a kind of experimental behavior was first demonstrated by Drexhage and co-workers in the 1960s 2,6 and recently was reported in monolayer emitters. 7,8 A metal surface with a roughness on the nanometer scale can confine incident light within regions far below the diffraction limit to generate modes of localized surface plasmons (LSPs), 2,9,10 leading to a strong light−matter interaction, which has drawn intense attention in the research of physics, chemistry, material, and life sciences. 11 −14 In general, the light−matter interaction is realizable in the vicinity of the metal nanoparticles.…”

“…A metal surface with a roughness on the nanometer scale can confine incident light within regions far below the diffraction limit to generate modes of localized surface plasmons (LSPs), ,, leading to a strong light–matter interaction, which has drawn intense attention in the research of physics, chemistry, material, and life sciences. − In general, the light–matter interaction is realizable in the vicinity of the metal nanoparticles. It includes enhancing or quenching fluorescence radiation and a cooperative emission of light by the ensemble of emitter dipoles near metal nanoparticles. ,− Considering a system of an emitter near metal particles, if small particles have a radius of R ≪ λ, the total electric field at the emitter site is the sum of the emitter’s own field E 0 and dipole field of particles E dip , E = E 0 + E dip . , Thus, it is proposed that in analogy with an interference effect when the emitter is in front of a planar interface, in some conditions the electric field superposition of | E 0 + E dip | 2 may generate destructive interference (decrease of ρ­( r ,ω)) to form metastable or dark states.…”

Plasmonically Enhanced Superradiance of Broken-Symmetry Diamond Color Center Arrays Inside Core-Shell Nanoresonators

“…The universal cooperative Purcell factor was also derived, which includes the plasmonic enhancement of individual emitters’ decay rates and the acceleration of the ensemble cooperative emission due to plasmonic correlations between them [ 45 , 46 ]. Inside a plasmonic nanocavity resulting in a nearly constant LDOS, the CET is proportional to the number of excited emitters, and its efficiency can be dynamically tuned in a wide range by varying the excitation power [ 47 ]. A unified theory was also developed for the compensation of loss accompanying the cooperative energy transfer and spasing [ 48 ].…”

“…It is a straightforward idea to enhance the emission of indistinguishable, symmetrically ordered emitters with a spherical nanoparticle. In the case of spherical metal nanoshells acting as concave nanoresonators around an embedded emitter ensemble, the resonance tunability can be exploited, and the strongly and uniformly enhanced EM-field inside the core can promote superradiance [ 46 , 47 , 53 , 54 ].…”