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Pumping-power-dependent photoluminescence angular distribution from an opal photonic crystal composed of monodisperse Eu^3+/SiO_2 core/shell nanospheres

Le Dac Tuyen, Jian Hung Lin, Cheng Yi Wu, Po-Tse Tai, Jau Tang, Le Quoc Minh, Hung‐Chih Kan, Chia‐Chen Hsu

Published Jun 25, 2012• 7 citations

Abstract

High quality opal photonic crystals (PhCs) were successfully fabricated by self-assembling of monodisperse Eu(3+)/SiO(2) core/shell nanospheres. Angular resolved photoluminescence (PL) spectra of a PhC sample were measured with different pumping powers, and its PL emission strongly depended on spectroscopic position of the photonic stop band and the optical pumping power. Suppression of the PL occurred in the directions where the emission lines aligned with the center of the photonic stop band. Suppression and enhancement of the PL were observed at low- and high-pumping powers, respectively, in the directions where the emission lines were located at the edges of the photonic stop band. When pumping power exceeded 6 µJ/pulse, a super-linear dependence was found between the pumping power and PL intensity. The dramatic enhancement of PL was attributed to the amplification of spontaneous emission resulted from the creation of large population inversion and the slow group velocity of the emitted light inside the PhC. The opal PhC provided highly angular-selective quasi-monochromatic PL output, which can be useful for a variety of optical applications.

DOI: 10.1364/oe.20.015418

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High quality opal photonic crystals (PhCs) were successfully fabricated by self-assembling of monodisperse Eu(3+)/SiO(2) core/shell nanospheres. Angular resolved photoluminescence (PL) spectra of a PhC sample were measured with different pumping powers, and its PL emission strongly depended on spectroscopic position of the photonic stop band and the optical pumping power. Suppression of the PL occurred in the directions where the emission lines aligned with the center of the photonic stop band. Suppression and enhancement of the PL were observed at low- and high-pumping powers, respectively, in the directions where the emission lines were located at the edges of the photonic stop band. When pumping power exceeded 6 µJ/pulse, a super-linear dependence was found between the pumping power and PL intensity. The dramatic enhancement of PL was attributed to the amplification of spontaneous emission resulted from the creation of large population inversion and the slow group velocity of the emitted light inside the PhC. The opal PhC provided highly angular-selective quasi-monochromatic PL output, which can be useful for a variety of optical applications.

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.

Angular distribution of photoluminescence of trivalent rare earth ions embedded inside three-dimensional opal and inverse opal photonic crystals is experimentally shown to be strongly modulated for the emission frequencies near the first and higher photonic stop-bands. Numerical simulations of fractional density of optical states also predict highly directional emission from photonic crystals with an ideal structure. Experimental results are shown to be in a good agreement with calculated angular dependencies of luminescence. However, better agreement between experimental and theoretical data requires smoothing of calculated dependencies, which can be attributed to the presence of structural imperfections in real photonic crystal samples.

SiO 2 inverse opals made with LaF 3:Tb 3+ nanoparticles were fabricated. The spontaneous emission lifetime of the 5 D 4 → 7 F 4 transition of Tb 3+ ions at 542 nm embedded in the SiO 2 inverse opal structure was determined. In contrast to an average lifetime of 2.8 ms in photonic crystals when the photoluminescence of the Tb 3+ envelop was located outside the photonic stop band, a lifetime of 4.0 ms was observed when the Tb 3+ photoluminescence fully overlaps with the photonic stop band in the inverse opal. The obtained results demonstrate that the photonic structure affects the spontaneous emission significantly, resulting in a 40% increase of the luminescence lifetime of Tb 3+ ions. In other words, the density of optical states is reduced at the emission frequency of Tb 3+ (i.e., 542 nm) which reduces the radiative rate constant.

The photonic dispersion, the group-velocity dispersion, the effective mass, refractive index, and the spectral distribution of the density of photonic states near the edge of the photonic stop band are numerically calculated in the one-dimensional model for photonic crystals based on synthetic opals. The fluorescence spectra of rhodamine 6G and 2,5-bis(2-benzoxazolyl)hydroquinone molecules infiltrated into a synthetic opal are measured. For both substances, it is observed that the spontaneous emission intensity in the range of the photonic stop band is appreciably suppressed. A blue shift of the fluorescence spectrum of rhodamine 6G molecules is revealed. Secondary emission of synthetic opals infiltrated with colloidal silver is observed in the Stokes range under excitation of opals by radiation at λ = 400 nm. The spectrum of the secondary emission is located in the range 450–590 nm, which contains the stop band and intervals near its edges.