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Physical review. B, Condensed matter

Coherent radiation scattering by resonant nanostructures

В. В. Климов, Vladilen S Letokhov

Published Jul 15, 2000• 11 citations
Publisher

Abstract

This paper deals with the scattering of radiation by resonant nanostructures, i.e., systems of like atoms arranged at distances much less than the wavelength of light. It is demonstrated that the quasistatic interaction of atoms in such nanostructures changes the eigenfrequency structure of the atoms forming the nanostructure and causes substantial alterations in the scattered light spectrum. With the plane polarization of the incident light wave, the spectrum can be singlet (two interacting atoms), doublet (three interacting atoms), and so on, depending on the number of atoms in the nanostructure. The potential possibility is discussed of using such resonant structures as ultrahigh-density ROM devices.

DOI
10.1103/physrevb.62.1639

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This paper deals with the scattering of radiation by resonant nanostructures, i.e., systems of like atoms arranged at distances much less than the wavelength of light. It is demonstrated that the quasistatic interaction of atoms in such nanostructures changes the eigenfrequency structure of the atoms forming the nanostructure and causes substantial alterations in the scattered light spectrum. With the plane polarization of the incident light wave, the spectrum can be singlet (two interacting atoms), doublet (three interacting atoms), and so on, depending on the number of atoms in the nanostructure. The potential possibility is discussed of using such resonant structures as ultrahigh-density ROM devices.
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.
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.
The existence of linear nonstationary optical resonances in a diatomic nanostructural object with a dipole-dipole atomic interaction has been proved. A new solution to the joint system of modified Bloch optical equations and nonlocal field equations is obtained for time intervals much shorter than the times of phase and energy relaxation. Formulas for effective polarizabilities of the object’s atoms, which have a set of dimensional resonances, are derived. The frequencies of these resonances significantly differ from the eigenfrequencies of the object’s atoms, and their properties depend on the interatomic distance, light-pulse duration, initial atomic inversions, and the orientation of the object’s axis relative to the direction of incidence of the external light wave.
In nanostructures with a high excitonic coherence, the interplay between the spatial structure of the excitonic wavefunction and that of the radiation field plays an essential role, causing drastic size effects in the optical response, such as size-resonant enhancement of the radiative decay rate and the nonlinear response and the interchange of quantized levels. This article discusses such peculiar optical effects based on the theoretical treatment beyond the long-wavelength approximation and demonstrates the possibility of designing novel photofunctions with the explicit use of the spatial structures of the radiation field.
For the combined system of equations of field and atomic variables for two different atoms in the ground state, a stationary solution is obtained, which takes into account their dipole-dipole interaction in the field of external emission. Atoms are treated as linear dipole oscillators with different natural frequencies and linear polarizabilities. Formulas for effective polarizabilities of atoms in a nanostructure object, whose dispersion properties substantially differ from the dispersion properties of isolated atoms in the region of their natural resonances, are obtained. It is found that a nanostructure object consisting of two different atoms has four dimensional resonances, whose frequencies strongly depend on the interatomic separation and the object orientation with respect to the direction of propagation of an external wave. Using interference from the coherent field of dipoles of a small object with a reference coherent wave in a certain plane of observation points in the wave region far from a small object, an optical hologram of a small object is obtained. It is shown by numerical experiments that a small object forms interference fringes with good contrast, which makes possible the use of optical quasi-resonant emission for the development of a nondestructive method of study of small objects.
On the basis of general theoretical results developed previously in [JETP 112, 246 (2011)], we analyze the reflection of quasiresonant light from a plane surface of dense and disordered ensemble of motionless point scatters. Angle distribution of the scattered light is calculated both for sss and ppp polarizations of the probe radiation. The ratio between coherent and incoherent (diffuse) components of scattered light is calculated. We analyze the contributions of scatters located at different distances from the surface and determine on this background the thickness of surface layer responsible for reflected beam generation. The inhomogeneity of dipole-dipole interaction near the surface is discussed. We study also dependence of total reflected light power on the incidence angle and compare the results of the microscopic approach with predictions of the Fresnel reflection theory. The calculations are performed for different densities of scatters and different frequencies of a probe radiation.