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Optics and Spectroscopy

Enhancement of hypersensitive transitions of rare-earth ions in the near field of nanoobjects

Konstantin K. Pukhov, Sergey K. Sekatskii

Published May 1, 2014• 3 citations

Abstract

The change of intensities of optical transitions of atoms, molecules, and their ions in the near field of nanoobjects is of interest for researchers from both basic and applied points of view. The concept of a near field was used as early as the 1960s to study the mechanisms of hypersensitive transitions of rare-earth (RE) ions. In this work, it is once more emphasized that, precisely for these transitions, changes in characteristics under the action of local properties of the medium are especially strong and, correspondingly, these transitions are especially promising for use. The Judd method for the calculation of the intensities of hypersensitive transitions of RE ions taking into account the inhomogeneous ligand field is extended to RE ions in the near field of nanoobjects. A simple analytical expression for the Judd-Ofelt intensity parameter Ω 2 for RE ions in the field of spherical nanoparticles of a subwavelength size is derived.

DOI: 10.1134/s0030400x14050191

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The change of intensities of optical transitions of atoms, molecules, and their ions in the near field of nanoobjects is of interest for researchers from both basic and applied points of view. The concept of a near field was used as early as the 1960s to study the mechanisms of hypersensitive transitions of rare-earth (RE) ions. In this work, it is once more emphasized that, precisely for these transitions, changes in characteristics under the action of local properties of the medium are especially strong and, correspondingly, these transitions are especially promising for use. The Judd method for the calculation of the intensities of hypersensitive transitions of RE ions taking into account the inhomogeneous ligand field is extended to RE ions in the near field of nanoobjects. A simple analytical expression for the Judd-Ofelt intensity parameter Ω 2 for RE ions in the field of spherical nanoparticles of a subwavelength size is derived.

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A new scheme to realize an abnormal dielectric response at optical wavelength is developed on the basis of two-level electronic transition of rare-earth ion doped crystals. Based on the semi-classical theory and the Judd—Ofelt theory, the electric dipole transition under a weak field is analyzed, and a general expression for the frequency-dependent dielectric constant is obtained. As an example, the permittivity of (Er x Y 1−x ) 3 Al 5 O 12 is calculated numerically in consideration of the transition between 4 I 15/2 and 4 F 9/2 . An optimized dielectric property with a negative real part and low absorption is achieved. This proposes a new mechanism for building extraordinary electromagnetic media at optical frequencies by using a quantum process.

The absorption of a single photon by the simultaneous excitation of two rare-earth ions was first reported by Varsanyi and Dieke in 1961.1 D. L. Dexter explained this unusual observation by including the electron-electron interactions (that also give rise to energy transfer) between the rare earth ions with perturbation theory.2 In the 70's Dexter became interested in electronic-vibrational coupling. A theory of two-center optical transitions was developed for a rare-earth ion weakly coupled to a high energy, internal vibrational mode of a near-lying ion.3 Using theoretical techniques that had been developed for rare-earth ion pairs, intensities and selection rules could be determined.

An analytical expression is proposed for the rate of radiative decay of excitations of optical centers in an ellipsoidal nanoparticle that is considerably smaller than the light wavelength ( a, b, c ≪ λ ) and is embedded in the surrounding medium. This expression is compared with the corresponding expression for a bulk crystal. The time of radiative decay in nanoparticles spherical in shape and identical in size (2 R ≪ λ ) is derived as a function of the dielectric characteristics of a nanocomposite and the nanoparticle volume fraction C in suspensions and aerosols. The expressions describing the emission and absorption cross sections in spherical nanoparticles are obtained. The experimentally measured and theoretically calculated decay times of metastable levels of rare-earth impurity ions in YAG and Y 2 O 3 crystalline nanoparticles are compared with those for bulk crystals with the same structure.