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Physica Scripta

Second-order correlation function of fluorescence from a few atoms near plasmonic surface

Mojtaba Moazzezi, Augustine M. Urbas, Vladimir P. Drachev, Yuri V. Rostovtsev

Published Feb 10, 2020• 1 citation
Publisher

Abstract

Abstract We have used a full quantum mechanical approach to study the second-order correlation function of a system of a few two-level atoms coupled via plasmons. By the usage of quantum regression theory we have developed a new model that allows us to fully investigate the dependence of photon bunching and anti-bunching effects to the interaction between atoms, fields and surrounding medium. Using Dicke basis for several atomic systems, we show that Dicke states can be coupled via various relaxation processes near plasmonic and metamaterial surfaces, and as a result, the second-order correlation function has various characteristic time scales related to the supperadiant and subradiant transitions and these prediction can be observed experimentally.

DOI
10.1088/1402-4896/ab5985

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Abstract We have used a full quantum mechanical approach to study the second-order correlation function of a system of a few two-level atoms coupled via plasmons. By the usage of quantum regression theory we have developed a new model that allows us to fully investigate the dependence of photon bunching and anti-bunching effects to the interaction between atoms, fields and surrounding medium. Using Dicke basis for several atomic systems, we show that Dicke states can be coupled via various relaxation processes near plasmonic and metamaterial surfaces, and as a result, the second-order correlation function has various characteristic time scales related to the supperadiant and subradiant transitions and these prediction can be observed experimentally.
This thesis is an attempt at studying quantum coherence effects coupled via plasmons. After introducing the quantum coherence in atomic systems in Chapter 1, we utilize it in Chapter 2 to demonstrate a new technique of detection of motion of single atoms or irons inside an optical cavity. By taking into account the interaction of coherences with surface plasmonic waves excited in metal nanoparticles, we provide a theoretical model along with experimental data in Chapter 3 to describe the modification of Raman spectra near metal nanoparticles. We show in chapter 4 that starting from two emitters, coupled via a plasmonic field, the symmetry breaking occurs, making detectable the simultaneous existence of the fast super-radiance and the slow sub-radiance emission of dye fluorescence near a plasmonic surface. In Chapter 5, we study the photon statistics of a group of emitters coupled via plasmons and by the use of quantum regression theorem, we provide a theoretical model to fully investigate the dependence of photon bunching and anti-bunching effects to the interaction between atoms, fields and surrounding mediums.
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 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 photon correlations of resonance fluorescence emitted by a degenerate two-level atom near a metal surface are studied. An intense nonmonochromatic optical laser drives a low-lying atomic transition, and the emitted fluorescence is detected by a photon counter. An expression for the spontaneous-decay operator is derived, and it appears that the various substates of the upper level have a different lifetime due to the presence of the surface, or equivalently, due to the loss of spherical symmetry. The temporal photon correlation function is then evaluated in terms of a photon-emission operator and the time-evolution operator for the atomic density matrix. The general theory is exemplified with a detailed elaboration of the jg{j}_{g}jg​=0\ensuremath{\rightarrow}je{j}_{e}je​=1 transition, for which the two-photon correlation is obtained explicitly as a function of the inverse lifetime A(h), depending on the atom-surface distance h, the laser linewidth, the detuning from resonance, and the dipole-coupling strength with the external field.
Abstract : The photon correlations of resonance fluorescence emitted by a degenerate two-level atom near a metal surface are studied. An intense non monochromatic optical laser drives a low lying atomic transition, and the emitted fluorescence is detected by a photon counter. An expression for the spontaneous decay operator is derived, and it appears that the various substates of the upper level have a different lifetime due to the presence of the surface, or equivalently, due to the loss of spherical symmetry. The temporal photon correlation function is then evaluated in terms of a photon-emission operator and the time evolution operator for the atomic density matrix. The general theory is exemplified with a detailed elaboration of the j sub g = 0 yields j sub e = 1 transition, for which the two-photon correlation is obtained explicitly as a function of the lifetime A(h), depending on the atom surface distance h, the laser linewidth, the detuning from resonance, and the dipole-coupling strength with the external field. Keywords: Photon correlations; Resonance fluorescence; Atom near metal surface; Loss of spherical symmetry; Substates; Different lifetimes.
We present a theoretical study of the resonance fluorescence of a four-level double-V\mathsf{V}V-type quantum emitter near a plasmonic nanostructure. The quantum system interacts with two orthogonal circularly polarized laser fields with the same frequency and intensity, but with different phases. For the plasmonic nanostructure we consider a two-dimensional array of metal-coated dielectric nanospheres. We show that the presence of the plasmonic nanostructure leads to strong modification of both the resonance fluorescence spectrum and the transition from antibunching to bunching for the fluorescent photons. In addition, we show that both the resonance fluorescence spectrum and the second-order correlation function are strongly phase-dependent so that the relative phase of laser fields can be used for the efficient control of the resonance fluorescence characteristics. The results are explained by using a dressed-state picture.