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CAOL . International Conference on Advanced Optoelectronics and Lasers

Luminescent photonic crystals

Sergey O. Klimonsky, Alexander S. Sinitskii, Vera V. Abramova, Svetlana V. Eliseeva, Juntao Li, Peiqing Zhang, Ming Li, Jianying Zhou, Yuri D. Tretyakov

Published Sep 1, 2008• 0 citations
Publisher

Abstract

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.

DOI
10.1109/caol.2008.4671900

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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.
The possibility of the directional enhancement of luminescence at frequencies near the edge of the second photonic bandgap of opal-type photonic crystals has been demonstrated both theoretically and experimentally. The directional patterns of radiation have been simulated by calculating the angular dependences of the density of optical states. The calculation results are compared to the experimental data obtained for the thin-film opals with terbium-containing complexes. Good agreement is achieved after the strong smoothing of the calculated curves; this smoothing is necessary because of the imperfection of the structure of actual samples.
We have performed angle-resolved measurements of spontaneous-emission spectra from laser dyes and quantum dots in opal and inverse opal photonic crystals. Pronounced directional dependencies of the emission spectra are observed: angular ranges of strongly reduced emission adjoin with angular ranges of enhanced emission. It appears that emission from embedded light sources is affected both by the periodicity and by the structural imperfections of the crystals: the photons are Bragg diffracted by lattice planes and scattered by unavoidable structural disorder. Using a model comprising diffuse light transport and photonic band structure, we quantitatively explain the directional emission spectra. This work provides detailed understanding of the transport of spontaneously emitted light in real photonic crystals, which is essential in the interpretation of quantum optics in photonic-band-gap crystals and for applications wherein directional emission and total emission power are controlled.
Photonic crystals based on silica colloidal crystals (artificial opals) exhibit pronounced stopbands for electromagnetic wave propagation and the corresponding modification of the photon density of states in the visible range. These spectrally selective features can be enhanced by impregnating opals with higher refractive materials like, e.g., polymers. Doping of these structures with dye molecules, semiconductor nanoparticles (quantum dots), and rare-earth ions provides a possibility to examine the challenging theoretical predictions of the inhibited spontaneous emission in photonic bandgap (PBG) materials. First experiments are discussed in which pronounced modification of spontaneous emission spectra and noticeable changes in decay kinetics were observed.
The photoluminescence of a dye embedded in the three-dimensional SnS2 inverted opal has been studied. Changes of the emission spectrum compared with the free-space dye emission was observed in the stop-band frequency range in accord with reflectance/transmission spectra of this photonic crystal. The angular-dependent component, due to the Bragg stop band, and the angular-independent component, which is, possibly, related to the minimum in the density of photon states, have been distinguished in the dye emission spectrum.
We present the first experiments that demonstrate strong angle-independent modification of spontaneous emission spectra from laser dyes in photonic crystals, made of inverse opals in titania. We show that both the fluorescence quantum efficiency and weak disorder play a key role in interpreting the experimental data. We compare the angle-independent emission spectra of dye in photonic crystals with spectra from such crystals with much smaller lattice spacings, for which emission is in the long wavelength limit. The ratio of emission power spectra shows inhibition of emission up to a factor ∼ 5 over a large bandwidth of 13% of the first order Bragg resonance frequency. The inhibition shifts to increasing wavelength with the lattice parameter, confirming the photonic nature of the phenomenon. The center frequency and bandwidth of the inhibition agree with the calculated total density of states, but the measured inhibition of the vacuum fluctuations is much larger. This result is confirmed by experiments using different dyes. We likely probe the strongly modulated local photonic density of states, due to the spatially nonuniform distribution of dye molecules over the unit cell.
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.