Fluorescence and Lasing in Liquid Crystalline Photonic Bandgap Materials

Wenyi Cao

Kent State University

Cholesteric liquid crystals (CLCs) and cholesteric blue phases (BPs) are one-dimensional and three-dimensional photonic bandgap (PGB) materials. In this work, fluorescence and lasing are experimentally studied in dye-doped CLC films and BPs, together with the calculations of density of states (DOS) in CLC films. The normal modes of light propagation in a CLC film in the direction along the helical axis have been obtained analytically, using transfer matrix method. Two normal modes are elliptically polarized and their DOS differ greatly. The value and wavelength of the largest DOS depend on the CLC film thickness. The fluorescence spectra of dye DCM in CLC films are greatly altered: suppressed in the stop band and enhanced at band edges with intensity oscillations. The altered fluorescence spectra are in good agreement with the calculated spectra from the DOS. The fluorescence lifetimes, however, have no measurable difference. At high dye concentration, the fluorescence intensity is quenched by the formation of dye excimers. Mirrorless lasing in CLC films has been studied systematically. The lasing wavelengths and thresholds are in good agreement with the calculated values from the DOS. The threshold is optimized over CLC film thickness and dye concentration. Lasing at defect modes has been observed in CLC composite structures. Photon-counting statistics confirms the transition from the incoherent fluorescence to coherent laser emission with increasing pump energy. The totally coherent emitting area is estimated from the diffraction pattern of the CLC laser emission. The structures of BPs are characterized through textures and reflection measurements. In BP I, the stimulated emission is due to the multiple reflection of the fluorescence by small BP I crystals. In large BP II single crystals, the fluorescence is altered and lasing occurs at edges of the reflection peak or at defect modes. Lasing in three dimensions has been observed for the first time in PGB materials, and understood in terms of coupling of orthogonal lasing modes by reciprocal lattice vector.

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