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Applied Physics Letters

Highly modified spontaneous emissions in YVO4:Eu3+ inverse opal and refractive index sensing application

Yongsheng Zhu, Wen Xu, Hanzhuang Zhang, Wei Wang, Tong Liu, Sai Xu, Zhipeng Sun, Hongwei Song

Published Feb 20, 2012• 33 citations
Publisher

Abstract

Here, we present strong modification of photonic crystals on the spontaneous emissions of Eu3+ ions in YVO4:Eu3+ inverse opal. It is interesting that due to the effect of local field, the 5D0-7FJ radiative lifetimes of Eu3+ ions in the PCs are all prolonged ∼2.5 times in contrast to the grinded reference (REF) in air, consistent with the empty cavity model. The photonic stop band and the radiative lifetime are both highly sensitive to the refractive index of the infiltrated solutions, in accordance with the real cavity model.

DOI
10.1063/1.3688167

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Here, we present strong modification of photonic crystals on the spontaneous emissions of Eu3+ ions in YVO4:Eu3+ inverse opal. It is interesting that due to the effect of local field, the 5D0-7FJ radiative lifetimes of Eu3+ ions in the PCs are all prolonged ∼2.5 times in contrast to the grinded reference (REF) in air, consistent with the empty cavity model. The photonic stop band and the radiative lifetime are both highly sensitive to the refractive index of the infiltrated solutions, in accordance with the real cavity model.
Engineering spontaneous emission by means of photonic crystals (PHC) is under extensive study. However PHC modification of line emissions of rare earth (RE) ions has not been thoroughly understood, especially in cases of weak opal PHCs and while emitters are well dispersed into dielectric media. In this study, poly-methyl methacrylate (PMMA) opal PHCs containing uniformly dispersed europium chelate were fabricated with finely controlled photonic stop band (PSB) positions. Measurements of luminescent dynamics and angle resolved/integrated emission spectra as well as numerical calculations of total densities of states (DOS) were performed. We determined that in weak opals, the total spontaneous emission rate (SER) of Σ(5)D(0)-(7)F(J) for Eu(3+) was independent of PSB positions but was higher than that of the disordered powder sample, which was attributed to higher effective refractive indices in the PHC rather than PSB effect. Branch SER of (5)D(0)-(7)F(2) for Eu(3+) in the PHCs, on the other hand, was spatially redistributed, suppressed or enhanced in directions of elevated or reduced optical modes, keeping the angle-integrated total unchanged. All the results are in agreement with total DOS approximation. Our paper addressed two unstudied issues regarding modified narrow line emission in weak opal PHCs: firstly whether PSB could change the SER of emitters and whether there exist, apart from PSB, other reasons to change SERs; secondly, while directional enhancement and suppression by PSB has been confirmed, whether the angle-integrated overall effect is enhancing or suppressing.
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.
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We have observed strongly modified spontaneous-emission spectra from laser dye in photonic crystals made of inverse opals in titania (TiO2).({\mathrm{TiO}}_{2}).(TiO2​). We identify stop bands with large relative widths of 1515%,15 comparable to the dyes' emission spectrum, and 7575%75 attenuation of the emission strength. For a wide range of angles, two stop bands are simultaneously manifested; their angle-dependent frequencies display an avoided crossing that is corroborated by reflectivity experiments. The edges of the stop bands agree well with band-structure calculations, but differ from simple Bragg diffraction as a result of multiple wave coupling. The strongly reduced dispersion of the Bloch modes likely causes a significant change in the density of states.
We report the first measurements, to our knowledge, of the modification of spontaneous emission rates of Eu3+ ions in the visible region owing to an absorbing medium. Precise levels of the absorption coefficient are introduced by codoping with different amounts of Nd3+. We use a binary glass system PbO-B2O3 as the host, the compositional variation of which leads to a change in the real part of the refractive index. Measured lifetimes are found to follow the real cavity model, and the data are analyzed by the model proposed by Scheel et al. [Phys. Rev. A 60, 4094 (1999)]. We give estimates of the parameter that is related to the radius of the cavity around Eu3+.
The study of Lamb shift plays a unique role in quantum electrodynamics because it provides an excellent test of the theory on photonic crystals (PCs). In this Letter, we present the first observation of large Lamb shift in the YBO(3):Eu(3+) inverse opals fabricated by the polystyrene templating method. In addition, it is very interesting to observe that the luminescent dynamics of Eu(3+) decayed with a faster power law (t(-3)), followed by a slower exponential process due to the coexistence of the diffusion field and the propagating field in the PCs.