光子带隙结构调制下发光体中的能量传递研究
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摘要
光子带隙结构(或称光子晶体)不仅产生出一大批新型材料和器件,也能够提供一种特殊的物理环境——具有波长尺度的介电周期场,利用这种特殊的物理环境可以调制发光材料的光学性质及之间的能量传递,而这种调制行为可以通过发光学实验进行研究。本论文拟在设计具有不同结构的光子晶体,研究三维光子带隙(赝带隙)对发光材料的光学性质及其之间能量传递的影响。
通过垂直沉积法制备了荧光染料掺杂的蛋白石光子晶体,采用稳态荧光光谱和时间分辨荧光光谱研究了光子带隙对染料之间的能量传递的调制。结果发现:当给体荧光素的发射峰和蛋白石光子晶体的光子带隙重叠时,在光子带隙的调制作用下,给体通过自发辐射传播释放光子的过程受到抑制,而通过与受体实现能量传递的过程成为给体从激发态回到基态的主要方式,光子带隙能增强荧光染料之间的能量传递,从而增强受体的荧光。
采用加速蒸发诱导共沉积法和溶胶-凝胶法制备了Tb1-XEuXPO4(X=0, 0.001, 0.0025)反蛋白石光子晶体,实验上首次研究了发光体基反蛋白石光子晶体中的能量传递。研究发现:当Tb3+的发射峰和反蛋白石的光子带隙重叠时,反蛋白石光子晶体的光子带隙增强了稀土离子之间的能量传递。同时,制备了具有(100)和(111)两种取向的TbPO4反蛋白石光子晶体,并首次研究了反蛋白石光子晶体(100)和(111)两种取向的光学性质。研究发现:(100)取向区域的光子带隙和(111)取向区域的光子带隙相比发生了蓝移;且反蛋白石光子晶体的(111)取向区域的光子带隙和Tb3+的发射峰重叠,由于光子带隙作用Tb3+的发光受到抑制。
采用离子交换方法制备了由聚苯乙烯微球构成的结晶化胶体阵列,并研究了结晶化胶体阵列中荧光染料之间的能量传递。证明了结晶化胶体阵列的光子带隙可以增强染料之间的能量传递效率。同时,在实验上首次研究了光子带隙和给体发射峰重叠程度不一样时,光子带隙对染料之间能量传递调制的差异;研究证实:给体的发射峰和光子带隙重叠越好,染料之间的能量传递受光子带隙的增强越强。采用原位聚合方法制备了荧光素掺杂的聚合结晶化胶体阵列,研究了聚合结晶化胶体阵列的发光性质。实验发现:聚合结晶化胶体阵列的光子带隙抑制了荧光素的发光。
The presence of the photonic band gap structure (referred as photonic crystals) not only leads to appearances of lots of new materials and devices but also creates a specific physical environment, i.e. a periodically dielectric field on the wave length scale.The optical property and energy transfer of photoelectric materials may be modulated by the periodically dielectric field on the wave length scale. In this paper, the photonic crystals with different structures have been designed and prepared, and the influences of the three dimensional photonic gap (pseudo-gap) on the optical behavior and energy transfer of the luminophors have been analyzed.
The dye-doped opal photonic crystal was prepared by the vertical deposition method. The energy transfer from Fluorescein to Rhodamine B was investigated through both stable fluorescence spectroscopy and time-resolved spectroscopy. The results show that when the emission peak of the donor Fluorescein overlaps the photonic band gap of the opal photonic crystals, the spontaneous emission of the donor is inhibited. The inhibition of the spontaneous emission of the donor results in a fact that the excitation state donor could returns to the ground state more easily by the energy transfer. That is, the energy transfer of dyes in the photonic crystals can be enhanced.
The Tb1-XEuXPO4 (X=0, 0.001, 0.0025) inverse opal photonic crystals were prepared by the accelerated evaporation induced self-assembly technique in combination with a sol-gel method. The photoluminescence of inverse opal was studied by fluorescence microscope. The energy transfer enhancement between rare earth ions was first observed experimentally in the inverse opal photonic crystals. Inverse opal photonic crystals of TbPO4 with coexistence of the (100) and (111) orientations were prepared. Optical and photoluminescence properties of the (100) and (111) orientations regions were investigated in TbPO4 inverse opals. It was found that the photonic bandgap of (100) orientation shifted to shorter wavelengths compared with that of (111) orientation in the inverse opals. The effect of the photonic bandgap on the spontaneous emission of the 5D4→7Fn transitions of Tb3+ was observed in the TbPO4 inverse opals with coexistence of the (100) and (111) orientations. Significant suppression of the emission was detected in the (111) orientation regions.
The ions exchange method was used to prepare crystalline colloidal arrays, in which the non-radiative energy transfer between fluorescence dyes was investigated. It has been verified that the energy transfer between fluorescence dyes can be enhanced by the photonic band gap of the crystalline colloidal arrays. Meanwhile, the energy transfer enhancement difference was first investigated when the overlaps between the photonic band gap and the donor’s emission peak was different. It has been revealed that the energy transfer and the radiative emission are related to the overlap between donor emission band and photonic band gap. The more overlapping between donor emission band and photonic band gap is, the more difficult the radiative emission is, contrarily, the stronger the energy transfer is.
The polymerized crystalline colloidal arrays were prepared by situ polymerization method. The influence of photonic band gap on photoluminescence of dyes was investigated. Suppression of the emission was observed if the photonic bandgap overlapped with the dyes emission band in the polymerized crystalline colloidal arrays.
通过垂直沉积法制备了荧光染料掺杂的蛋白石光子晶体,采用稳态荧光光谱和时间分辨荧光光谱研究了光子带隙对染料之间的能量传递的调制。结果发现:当给体荧光素的发射峰和蛋白石光子晶体的光子带隙重叠时,在光子带隙的调制作用下,给体通过自发辐射传播释放光子的过程受到抑制,而通过与受体实现能量传递的过程成为给体从激发态回到基态的主要方式,光子带隙能增强荧光染料之间的能量传递,从而增强受体的荧光。
采用加速蒸发诱导共沉积法和溶胶-凝胶法制备了Tb1-XEuXPO4(X=0, 0.001, 0.0025)反蛋白石光子晶体,实验上首次研究了发光体基反蛋白石光子晶体中的能量传递。研究发现:当Tb3+的发射峰和反蛋白石的光子带隙重叠时,反蛋白石光子晶体的光子带隙增强了稀土离子之间的能量传递。同时,制备了具有(100)和(111)两种取向的TbPO4反蛋白石光子晶体,并首次研究了反蛋白石光子晶体(100)和(111)两种取向的光学性质。研究发现:(100)取向区域的光子带隙和(111)取向区域的光子带隙相比发生了蓝移;且反蛋白石光子晶体的(111)取向区域的光子带隙和Tb3+的发射峰重叠,由于光子带隙作用Tb3+的发光受到抑制。
采用离子交换方法制备了由聚苯乙烯微球构成的结晶化胶体阵列,并研究了结晶化胶体阵列中荧光染料之间的能量传递。证明了结晶化胶体阵列的光子带隙可以增强染料之间的能量传递效率。同时,在实验上首次研究了光子带隙和给体发射峰重叠程度不一样时,光子带隙对染料之间能量传递调制的差异;研究证实:给体的发射峰和光子带隙重叠越好,染料之间的能量传递受光子带隙的增强越强。采用原位聚合方法制备了荧光素掺杂的聚合结晶化胶体阵列,研究了聚合结晶化胶体阵列的发光性质。实验发现:聚合结晶化胶体阵列的光子带隙抑制了荧光素的发光。
The presence of the photonic band gap structure (referred as photonic crystals) not only leads to appearances of lots of new materials and devices but also creates a specific physical environment, i.e. a periodically dielectric field on the wave length scale.The optical property and energy transfer of photoelectric materials may be modulated by the periodically dielectric field on the wave length scale. In this paper, the photonic crystals with different structures have been designed and prepared, and the influences of the three dimensional photonic gap (pseudo-gap) on the optical behavior and energy transfer of the luminophors have been analyzed.
The dye-doped opal photonic crystal was prepared by the vertical deposition method. The energy transfer from Fluorescein to Rhodamine B was investigated through both stable fluorescence spectroscopy and time-resolved spectroscopy. The results show that when the emission peak of the donor Fluorescein overlaps the photonic band gap of the opal photonic crystals, the spontaneous emission of the donor is inhibited. The inhibition of the spontaneous emission of the donor results in a fact that the excitation state donor could returns to the ground state more easily by the energy transfer. That is, the energy transfer of dyes in the photonic crystals can be enhanced.
The Tb1-XEuXPO4 (X=0, 0.001, 0.0025) inverse opal photonic crystals were prepared by the accelerated evaporation induced self-assembly technique in combination with a sol-gel method. The photoluminescence of inverse opal was studied by fluorescence microscope. The energy transfer enhancement between rare earth ions was first observed experimentally in the inverse opal photonic crystals. Inverse opal photonic crystals of TbPO4 with coexistence of the (100) and (111) orientations were prepared. Optical and photoluminescence properties of the (100) and (111) orientations regions were investigated in TbPO4 inverse opals. It was found that the photonic bandgap of (100) orientation shifted to shorter wavelengths compared with that of (111) orientation in the inverse opals. The effect of the photonic bandgap on the spontaneous emission of the 5D4→7Fn transitions of Tb3+ was observed in the TbPO4 inverse opals with coexistence of the (100) and (111) orientations. Significant suppression of the emission was detected in the (111) orientation regions.
The ions exchange method was used to prepare crystalline colloidal arrays, in which the non-radiative energy transfer between fluorescence dyes was investigated. It has been verified that the energy transfer between fluorescence dyes can be enhanced by the photonic band gap of the crystalline colloidal arrays. Meanwhile, the energy transfer enhancement difference was first investigated when the overlaps between the photonic band gap and the donor’s emission peak was different. It has been revealed that the energy transfer and the radiative emission are related to the overlap between donor emission band and photonic band gap. The more overlapping between donor emission band and photonic band gap is, the more difficult the radiative emission is, contrarily, the stronger the energy transfer is.
The polymerized crystalline colloidal arrays were prepared by situ polymerization method. The influence of photonic band gap on photoluminescence of dyes was investigated. Suppression of the emission was observed if the photonic bandgap overlapped with the dyes emission band in the polymerized crystalline colloidal arrays.
引文
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