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International Conference Laser Optics (ICLO)

Microscopic approach to calculation of the spontatneous decay of an excited atom located near an atomic cluster

A. S. Kuraptsev, Igor M. Sokolov

Published Jun 1, 2014• 0 citations
Publisher

Abstract

We report the microscopic method for the calculation of the spontaneous decay of an excited atom located near a nanoparticle. The spontaneous decay dynamics, the atomic transition line shape as well as its shift have been analyzed. Different form, sizes and densities of the atomic cluster have been considered.
DOI
10.1109/lo.2014.6886379

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The optical properties of an atom located near a cluster of two arbitrarily arranged nanospheres of an arbitrary composition are studied. Changes in the spontaneous decay rates of excited states and emission frequency shifts are considered for different orientations of the dipole moment and different positions of the atom with respect to the cluster. It is shown that a two-nanosphere cluster can be used to control efficiently the spontaneous decay rates of excited states of the atom by changing the distance between spheres. It is found that spontaneous decay rates of the excited states of an atom located between silver nanospheres and having the dipole moment directed along the axis connecting the centres of spheres can increase by a factor of 10 5 and more when nanospheres are brought closer together.
The effect of nanobodies, i.e., the bodies whose size is small compared to the emission wavelength, on spontaneous emission of an atom located near them is considered. The results of calculations performed within the framework of quantum and classical electrodynamics are presented both in analytic and graphical forms and can be readily used for planning experiments and analysis of experimental data. It is shown that nanobodies can be used to control efficiently the rate of spontaneous transitions. Thus, an excited atom located near a nanocylinder or a nanospheroid pole, whose transition dipole moment is directed normally to the nanobody surface, can decay with the rate that is tens and hundreds times higher than the decay rate in a free space. In the case of some (negative) dielectric constants, the decay rate can increase by a factor of 10 5 —10 6 and more. On the other hand, the decay of an excited atom whose transition dipole moment is directed tangentially to the nanobody surface substantially slows down. The probability of nonradiative decay of the excited state is shown to increase substantially in the presence of na-nobodies possessing losses.
In the frames of quantum electrodynamics, the behavior of spontaneous decay is investigated for a single two-level atom embedded into a microscopic object (cluster). The transition frequency of cluster atoms is supposed to be considerably detuned from the transition frequency of decaying atom. The consideration is performed on the base of fully microscopic quantum-electrodynamical approach with simultaneous solution of Heisenberg equations for atomic and quantum field operators. The special attention is paid to the investigation of renormalization of spontaneous emission rate due to proper account of discrete structure of medium. The formula for decay rate is obtained without using the notion of refractive index. It is obtained that spontaneous decay strongly depends on the geometrical arrangement of atoms in microstructure. For some form of clusters, decay rate is found to be considerably large compared to its vacuum value that is not the case for macroscopically large dielectrics.
We report the results of numerical modelling of emission of a two-level atom near a metal nanoparticle under resonant interaction of light with plasmon modes of the particle. Calculations have been performed for different polarisations of light by a dipole approximation method and a complex multipole method. Depending on the distance between a particle and an atom, the contribution of the nonradiative process of electron tunnelling from a two-level atom into a particle, which is calculated using the quasi-classical approximation, has been taken into account and assessed. We have studied spherical gold and silver particles of different diameters . The rates of electron tunnelling and of spontaneous decay of the excited atomic state are found. The results can be used to develop nanoscale plasmonic emitters, lasers and photodetectors.