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Journal of the Optical Society of America B

Influence of local-field effects on the radiative lifetime of liquid suspensions of Nd:YAG nanoparticles

Ksenia Dolgaleva, Robert W. Boyd, Peter W. Milonni

Published Feb 15, 2007• 52 citations
Publisher

Abstract

We measured the radiative lifetime of Nd:YAG nanopowder with an average particle size of 20nm suspended in different organic and inorganic liquids. To extract information regarding local-field effects, we fitted the experimental data to three different local-field models: the virtual-cavity (or Lorentz) model, the real-cavity model, and the no-local-field-effects model. The real-cavity model and the no-local-field-effects model can both be adequately fitted to our experimental results, while the virtual-cavity model can be ruled out.

DOI
10.1364/josab.24.000516

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We measured the radiative lifetime of Nd:YAG nanopowder with an average particle size of 20nm suspended in different organic and inorganic liquids. To extract information regarding local-field effects, we fitted the experimental data to three different local-field models: the virtual-cavity (or Lorentz) model, the real-cavity model, and the no-local-field-effects model. The real-cavity model and the no-local-field-effects model can both be adequately fitted to our experimental results, while the virtual-cavity model can be ruled out.
The radiative lifetime of an emitter (such as a luminescent ion) is affected not only by the properties of the emitter itself but also by the dielectric properties of the surrounding media. The fluctuation of the local electrical field caused by random distribution of polarized luminescent-ion-containing nanoparticles in media leads to the fluctuation of radiative lifetime of luminescent ions. Lifetime fluctuation has been calculated analytically by considering this effect. The results show that the fluctuation of radiative lifetime is not negligible and can be shown and observed in future experiments.
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.
Behavior of radiation of Nd:YAP and Nd:YAG in a resonator with extremely low Q-value have been studied. The light pulses of the form discrete spikes around 1.08 micrometers have been observed using a relatively low pumping energies in Nd:YAP. The formation of these pulses has threshold character. Additional measurement such as second harmonic generation, far field distribution and spectral behavior have shown that emitted pulses have a typical laser character. Derived value of threshold gain parameter with material losses (g0 - (alpha) ) for threshold energy is 0.581 cm-1. No similar effect was observed for Nd:YAG, even for four timeshigher value of threshold energy than Nd:YAP. Obtained results demonstrate the cooperative effects of Nd3+ ions in Nd:YAP through a correlation between electromagnetic and crystal field.
In order to discriminate between the two macroscopic models for the dependence of the spontaneous emission rates of emitters on the refractive indices of the surrounding optical dielectric media, i.e., the local-field effect, Eu3+ activated glass samples with a range of different refractive indices were prepared for the measurements of photoluminescence emission spectrum, luminescent decay rate and refractive index. Detail analyses indicate that the local-field effect on the spontaneous emission rates follows the virtual-cavity model derived by assuming the doped luminescent ions do not disturb the optical dielectric media.