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Optics and Spectroscopy

Metastructural systems of activated nanospheres and optical near-field resonances

Oleg N. Gadomsky, Aleksei S. Kadochkin

Published Feb 1, 2005• 1 citation
Publisher

Abstract

The near-field interaction of two spherical nanoparticles containing dense ensembles of two-or multilevel atoms in an external field of optical low-intensity radiation is shown to result in the formation of resonances whose frequencies differ considerably from the transition frequencies in the spectrum of the interacting atoms. Optical near-field resonances are shown to play an important role in metastructural systems composed of activated nanospheres. The reflectance of a metastructural system of activated nanospheres oriented along a certain direction depends strongly on the polarization and the frequency of external radiation, as well as on the concentration of impurity atoms inside the nanospheres and on their sizes.

DOI
10.1134/1.1870070

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The near-field interaction of two spherical nanoparticles containing dense ensembles of two-or multilevel atoms in an external field of optical low-intensity radiation is shown to result in the formation of resonances whose frequencies differ considerably from the transition frequencies in the spectrum of the interacting atoms. Optical near-field resonances are shown to play an important role in metastructural systems composed of activated nanospheres. The reflectance of a metastructural system of activated nanospheres oriented along a certain direction depends strongly on the polarization and the frequency of external radiation, as well as on the concentration of impurity atoms inside the nanospheres and on their sizes.
The existence of optical size resonances in atomic nanostructures is proved. The properties of optical size resonances strongly depend on the interatomic distances and on the polarization of an external radiation field. The properties of linear and nonlinear size resonances are considered in the case of two-dimensional nanostructures. The linear optical size resonances are described based on a closed system of equations for dipole oscillators and nonlocal field equations taking into account the dipole-dipole interactions of atoms in the radiation field. Using a stationary solution to these equations, it is demonstrated that two isotropic atoms with definite intrinsic frequencies form an anisotropic system in the radiation field, possessing two or four size resonances depending on whether the component atoms are identical or different. The nanostructure composed of two different atoms possesses two size resonances with positive dispersion and two other resonances with negative dispersion. The frequencies of the size resonances significantly differ from the intrinsic frequencies of isolated atoms entering into the nanostructure. By changing the angle of incidence of the external wave, it is possible to excite various size resonances. The properties of nonlinear optical size resonances excited by an intense radiation field were theoretically and numerically studied using the modified Bloch equations and nonlocal field equations. Dispersion relationships for the nonlinear resonances were derived and the inversion properties of atoms in the nanostructure were studied for various polarizations of the external optical wave.
Modification of the resonance fluorescence spectrum of a two-level atom driven by a monochromatic field in the close proximity of a plasmonic nanostructure (metal sphere) is studied in detail. It is shown that one can control this spectrum by varying several key parameters: (i) the radius of the nanosphere, (ii) polarization of the incident radiation, and (iii) the atom's location around the nanosphere (its radial coordinate and polar angle in the spherical coordinate system). These parameters affect the local field enhancement and the modification of the radiative decay rate of the atom interacting with the nanosphere, which leads to modification of the resonance fluorescence spectrum of the atom (e.g., frequency shift of the satellite lines in the Mollow-type triplet, widths of the lines, and the spectrum intensity) by contrast with that in free space. The permittivity of the metal the nanosphere is made of is also an additional parameter, which defines the nonradiative decay. The latter in combination with other parameters allows continuous control of the transition from resonance fluorescence enhancement to its quenching.
It has been shown that nonlinear near-field optical resonances occur in diatomic nanostructures consisting of identical or different two-level atoms in the presence of a radiation field when the dipole-dipole interaction is taken into account. The frequencies of these resonances depend strongly on the intensity of the external optical radiation, on the initial conditions, on the polarization of the external field with respect to the axis of the nanostructure, and on the interatomic distance. The interatomic interaction is taken into account beyond perturbation theory. For this reason, the effective polarizabilities of the atoms of the nanostructure are expressed in terms of the polynomials of both the interatomic distance and the electric field strength of the external optical wave. A “falling tower” effect that is caused by the nonlinear behavior of the local dipole moments of atoms in the nanostructure is predicted.
This review is devoted to the study of effects of quantum optics in nanostructures. The mechanisms by which the rates of radiative and nonradiative decay are modified are considered in the model of a two-level quantum emitter (QE) near a plasmonic nanoparticle (NP). The distributions of the intensity and polarization of the near field around an NP are analyzed, which substantially depend on the polarization of the external field and parameters of plasmon resonances of the NP. The effects of quantum optics in the system NP + QE plus external laser field are analyzed-modification of the resonance fluorescence spectrum of a QE in the near field, bunching/antibunching phenomena, quantum statistics of photons in the spectrum, formation of squeezed states of light, and quantum entangled states in these systems.
We have solved a boundary-value problem for a ball probe interacting with a flat dielectric surface in an external optical radiation field. This interaction gives rise to the optical size resonance at frequencies significantly different from the natural frequencies of two-level atoms both in the medium and in the probe with allowance for the local field corrections. These resonances depend significantly on the distance from the probe center to the surface, on the ball probe size, on the concentration of two-level atoms in the probe and in the medium, on the spectral line width, and on the atomic inversion. The field strengths inside and outside the ball probe and a semiinfinite dielectric medium have been calculated in the near-field and wave zones. It is shown that the proposed electrodynamic theory of optical near-field microscopy agrees with the results of experimental measurements.
It is shown that magnetic interaction of closely spaced atoms is an electromagnetic field leads to the formation of dimensional magnetic resonances with small widths and frequencies that differ considerably from the frequency of the magnetic resonance of an isolated atom and depend strongly on the interatomic distance and polarization of the external field. The interactions between two identical atoms and between two different atoms are considered with allowance for spin and orbital quantum transitions. Dimensional magnetic resonances in a diatomic nanostructure system are studied on the basis of a non-perturbation-theory-based solution to a system of equations for the field and atomic variables.