磷光敏化荧光的白色有机电致发光器件的研究
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摘要
摘要：有机电致发光作为下一代的显示和照明技术一直是广大的光电研究人员关注的焦点,但是常规有机电致发光器件25%的量子效率限制成为一个不可突破理论极限。随着可以实现三线态激子电致发光的磷光材料的问世,为突破这一理论极限提供了可能,利用磷光材料制备的有机电致发光器件的发光效率在不断地提高,但是其在大电流下的电致磷光效率迅速下降问题成为影响其使用的一个瓶颈。为解决三线态激子湮灭导致的磷光材料掺杂的电致发光器件在大电流密度时发光效率的迅速下降问题,本博士论文利用荧光与磷光材料共掺杂的方式,通过能量传递的方式来降低三线态激子寿命,减少三线态激子湮灭效应。并在此基础上,通过选择与磷光材料在颜色上匹配的荧光材料,同时对发光器件的结构进行了合理的设计,最终实现了高亮度的白色电致发光器件,并对磷光敏化荧光相关的机理问题进行了详细的研究。磷光敏化荧光电致发光器件在电激发下具有更大激子形成截面,同时具有短的三线态激子寿命,会大大降低在大电流时三线态激子湮灭的发生,对提高器件发光效率具有显著作用。本文一共分为五章,第一章总结了最新的关于有机白光电致发光器件的研究进展,并介绍了相关的发光材料和器件的工作原理以及有机电致发光的研究和测试方法。第二至四章是本论文的研究部分,具体内容如下：
第二章,首先,通过对于(Poly(9-vinylcarbazole))(PVK):Bis(2,4-difluorophenylpyridinato)(Fir6):rubrene薄膜的吸收、光致激发以及稳态光致发射光谱的研究,确定了Fir6与rubrene间能量传递过程对于薄膜的发光性质具有非常重要的作用,并通过激子动力学模型对其作用进行了说明。然后,利用瞬态发光测量技术对PVK:Fir6:rubrene薄膜的瞬态发光衰减曲线进行了研究,确定Fir6与rubrene间能量传递传递过程可以有效的降低Fir6的三线态激子寿命,证明了利用磷光材料与荧光材料之间的能量传递作用来解决磷光材料电致发光效率在大电流迅速下降问题的可行性。通过研究Fir6与rubrene间能量传递速率与rubrene浓度间的关系说明了他们之间的能量传递过程是以分子间电偶极相互作用的Foster能量传递作用为主。最后,通过电致发光器件发光效率的研究证实了Fir6与rubrene间能量传递可以改善Fir6的电致发光效率随电流下降的问题,并得到了器件效率整体的提高。说明了磷光敏化荧光的电致发光是提高大电流下电致发光效率的有效手段。
第三章,本章主要对在磷光荧光双掺杂的电致发光器件中电致发光颜色随电压产生飘移的问题进行了研究。通过分析,我们排除了电场引起的激子复合区域的移动以及荧光掺杂客体饱和而引起颜色随电压飘移的可能。通过对PVK:Fir6:rubrene(100:10:0.3in wt.)薄膜的电调制下的稳态以及瞬态光致发光的研究,确定了Fir6与rubrene间Dexter能量传递作用随电场而得到增强的效应是导致发光器件颜色随电压飘移的一个重要原因。我们还发现掺杂客体对于载流子的直接俘获作用也是造成PVK:Fir6:rubrene薄膜电致发射光谱随电压变化的另一重要原因。最后,我们进行了利用电致激基缔合物来避免在双掺杂器件中两掺杂客体间能量传递的作用而实现白色发光的尝试并且通过perylene与(1,1-Bis[4-[N,N'-di(p-tolyl)amino]phenyl]cyclohexane)(TAPC)双掺杂的PVK聚合物发光器件实现了白光的发射。
第四章,我们进行了利用绿色磷光材料(fac-tris (2-phenylpyridine) iridium (Ir(ppy)3)来敏化荧光材料4-(dicyanomethylene)-2-t-butyl-6-(1,1,7,7-tetramethyljulolidyl-9-enyl)-4Hpyran (DCJTB)的研究,通过对器件结构上的设计,实现了对在电激发下所产生的单线态和三线态激子进行管理的办法来达到获得高亮度的白色电致发光器件的目的。通过对PVK:Ir(ppy)3:DCJTB薄膜的光致发光、三线态激子寿命和电致发光器件的发光特性的研究证实了Ir(ppy)3对于DCJTB可以实现良好的敏化效果。根据合成白光在颜色方面的考虑,选择了掺杂浓度为PVK:Ir(ppy)3:DCJTB为(100:5:0.4in wt.)的掺杂聚合物薄膜与N,N'-diphenyl-N,N'-bis(1-naphthyl)-1,1'-bipheny1-4,4"-diamine(NPB)蓝色荧光层搭配来实现白光。利用2,9-Dimethyl-.4,7-diphenyl-1,10-phenanthroline (BCP)的空穴阻挡作用实现对激子复合区域的控制,同时利用单线态激子与三线态激子不同长度的扩散距离,通过结构为ITO/PEDOT:PSS (30nm)/PVK:Ir(ppy)3:DCJTB (100:5:0.4in wt.)(60nm)/NPB(4nm)/BCP(10nm)/Alq3(20nm)/LiF(1nm)/Al(100nm)的电致发光器件实现了对于单线态和三线态激子管理的目的,并获得了白色发光,其亮度为8700cd/m2,最大流明效率为4lm/W。
第五章,是结论与未来工作展望。通过上面的研究,我们得到以下结论：1,确定通过磷光敏化荧光可以改善大电流情况电致磷光效率迅速下降的问题并实现了器件整体效率的提高。2,确定了电场诱导的能量传递增强与荧光材料对载流子直接俘获作用会影响电致发射光谱的稳定性。3,通过对器件结构的设计,实现了器件的激子管理并获得了高亮度的白光发射。我们将在以下两个方面开展进一步研究。材料方面,需要找到成膜性更好能级更加匹配的聚合物主体以便可以获得更加优化的磷光敏化荧光。器件制备方面,需要通过器件结构的设计与制备方法的改进来改善器件发光的色稳定性问题。
ABSTRACT: Organic light emitting device (OLED) has been attracting a great deal of attention for its potential to be the next generation technology for lighting and display. However, this theoretical upper limit is only25%of the corresponding quantum efficiency for electroluminescence from the regular OLED, which limits the development of OLED. As phosphorescent materials were presented, it becomes possible to use triplet state to realize high efficient phosphorescence, which provides the possibility to break through the theoretical limit of25%quantum. Although the use of phosphorescent materials can significantly increase the efficiency of OLED, the rolling off of electrophosphorescent efficiency at high current density has been denounced. Some investigate shows that the rolling off of efficiency results from triplet-triplet annihilation at high current density. For sake of finding out the ways to reduce the rolling off of electrophosphorescent efficiency, in this dissertation, phosphorescent material to fluorescent material were codoped the host to reduce the lifetime of triplet state and the triplet-triplet annihilation through the energy transfer from phosphorescent material to fluorescent material. By the way, some tries to realize the high luminance white OLED were made by choosing the appropriate fluorescent dopant which could emit complementary color of phosphorescent dopant and designing a appropriated device structure. We investigated the relative principle for phosphorescent sensitized fluorescence in detail as well. The phosphorescent sensitized OLED provides a ability to enhance the efficiency of OLED for their larger exciton cross section and less triplet lifetime can prevent the triplet-triplet annihilation. The dissertation consists of five chapters. In the first chapter, we summarize the recent progress of White OLED and introduce the relative organic light emitting material, operation principle of device and the method of researching and measuring of OLED. In the other chapters, we present the detail of our research. The detail is listed as below.
In chapter2, we verified the determined effect of the energy transfer from Fir6to rubrene on the emission from PVK:Fir6:rubrene co-dopant OLED by analyzing the absorption spectrum, excited spectrum and steady state photo-luminescence spectrum. We also proved the viability of reducing the efficiency rolling off of electrophosphorescentce at high current density by utilizing Foster energy transfer from Fir6to rubrene to reduce triplet lifetime of Fir6and realized the efficiency enhancement of phosphorescent OLED. Phosphorescent sensitized fluorescent luminescence could be a effective way to enhance the efficiency of phosphorescent OLED at high current density.
In chapter3, we put our attention on the color-shift problem in phosphorescent and fluorescent co-dopants OLED. At first, we exclude that the shift of recombination zone under electric field and saturation of fluorescent co-dopant at high current density result in the color-shift. The electric field enhanced Dexter energy transfer from Fir6to rubrene could be responsible for the color-shift problem by analyzing the electric modulated PL spectrum and transient PL of OLED based on PVK:Fir6:rubrene. As well we found out that carrier trapping effect of rubrene is important for the spectrum-shift as voltage increasing. By avoiding the energy transfer between the two dopants in co-dopants OLED to prevent the color-shift, we realized the white emitting by combing the emission from electromer of TAPC monomer of perylene.
In chapter4, We obtained a high luminance white OLED depending on the structure designing with excitons management, in which green phosphorescent material (Ir(ppy)3) sensitize the red fluorescent material(DCJTB). For the sake of improving the chromaticity dependence of white color on the applied voltage, PVK:Ir(ppy)3:DCJTB (100:5:0.4in wt.) polymer was chosen to combine with NPB blue fluorescent material to obtain the white light emitting. At last, we realized the excitons management and obtained the white OLED with8700cd/m2maximum luminance and41m/w luminous efficiency by controlling the recombination zone utilizing the device structure of ITO/PEDOT:PSS (30nm)/PVK:Ir(ppy)3:DCJTB (100:5:0.4in wt.)(60nm)/NPB(4nm)/BCP(10nm)/Alq3(20nm)/LiF(1nm)/Al(100nm).
In chapter5, We present the conclusions and future work。Upon above research, we could conclude that1, The rolling off of electrophosphorescent efficiency at high current density could be relieved by phosphorescent sensitized fluorescence and efficiency enhancement of OLED could be achieved.2,The color stability could be affected by the electric field enhanced Dexter energy transfer from Fir6to rubrene and carrier trapping effect of rubrene.3, The exciton management and highly luminance white OLED was realized by the structure design of OLED. In my opinion, there are something more to research. The one is to achieve better phosphorescent sensitized fluorescence, the polymer host which have better film-forming and more appropriate energy bandgap was needed. The other one is the research on architecture and fabrication of OLED is needed to improve the color stability of OLED.
第二章,首先,通过对于(Poly(9-vinylcarbazole))(PVK):Bis(2,4-difluorophenylpyridinato)(Fir6):rubrene薄膜的吸收、光致激发以及稳态光致发射光谱的研究,确定了Fir6与rubrene间能量传递过程对于薄膜的发光性质具有非常重要的作用,并通过激子动力学模型对其作用进行了说明。然后,利用瞬态发光测量技术对PVK:Fir6:rubrene薄膜的瞬态发光衰减曲线进行了研究,确定Fir6与rubrene间能量传递传递过程可以有效的降低Fir6的三线态激子寿命,证明了利用磷光材料与荧光材料之间的能量传递作用来解决磷光材料电致发光效率在大电流迅速下降问题的可行性。通过研究Fir6与rubrene间能量传递速率与rubrene浓度间的关系说明了他们之间的能量传递过程是以分子间电偶极相互作用的Foster能量传递作用为主。最后,通过电致发光器件发光效率的研究证实了Fir6与rubrene间能量传递可以改善Fir6的电致发光效率随电流下降的问题,并得到了器件效率整体的提高。说明了磷光敏化荧光的电致发光是提高大电流下电致发光效率的有效手段。
第三章,本章主要对在磷光荧光双掺杂的电致发光器件中电致发光颜色随电压产生飘移的问题进行了研究。通过分析,我们排除了电场引起的激子复合区域的移动以及荧光掺杂客体饱和而引起颜色随电压飘移的可能。通过对PVK:Fir6:rubrene(100:10:0.3in wt.)薄膜的电调制下的稳态以及瞬态光致发光的研究,确定了Fir6与rubrene间Dexter能量传递作用随电场而得到增强的效应是导致发光器件颜色随电压飘移的一个重要原因。我们还发现掺杂客体对于载流子的直接俘获作用也是造成PVK:Fir6:rubrene薄膜电致发射光谱随电压变化的另一重要原因。最后,我们进行了利用电致激基缔合物来避免在双掺杂器件中两掺杂客体间能量传递的作用而实现白色发光的尝试并且通过perylene与(1,1-Bis[4-[N,N'-di(p-tolyl)amino]phenyl]cyclohexane)(TAPC)双掺杂的PVK聚合物发光器件实现了白光的发射。
第四章,我们进行了利用绿色磷光材料(fac-tris (2-phenylpyridine) iridium (Ir(ppy)3)来敏化荧光材料4-(dicyanomethylene)-2-t-butyl-6-(1,1,7,7-tetramethyljulolidyl-9-enyl)-4Hpyran (DCJTB)的研究,通过对器件结构上的设计,实现了对在电激发下所产生的单线态和三线态激子进行管理的办法来达到获得高亮度的白色电致发光器件的目的。通过对PVK:Ir(ppy)3:DCJTB薄膜的光致发光、三线态激子寿命和电致发光器件的发光特性的研究证实了Ir(ppy)3对于DCJTB可以实现良好的敏化效果。根据合成白光在颜色方面的考虑,选择了掺杂浓度为PVK:Ir(ppy)3:DCJTB为(100:5:0.4in wt.)的掺杂聚合物薄膜与N,N'-diphenyl-N,N'-bis(1-naphthyl)-1,1'-bipheny1-4,4"-diamine(NPB)蓝色荧光层搭配来实现白光。利用2,9-Dimethyl-.4,7-diphenyl-1,10-phenanthroline (BCP)的空穴阻挡作用实现对激子复合区域的控制,同时利用单线态激子与三线态激子不同长度的扩散距离,通过结构为ITO/PEDOT:PSS (30nm)/PVK:Ir(ppy)3:DCJTB (100:5:0.4in wt.)(60nm)/NPB(4nm)/BCP(10nm)/Alq3(20nm)/LiF(1nm)/Al(100nm)的电致发光器件实现了对于单线态和三线态激子管理的目的,并获得了白色发光,其亮度为8700cd/m2,最大流明效率为4lm/W。
第五章,是结论与未来工作展望。通过上面的研究,我们得到以下结论：1,确定通过磷光敏化荧光可以改善大电流情况电致磷光效率迅速下降的问题并实现了器件整体效率的提高。2,确定了电场诱导的能量传递增强与荧光材料对载流子直接俘获作用会影响电致发射光谱的稳定性。3,通过对器件结构的设计,实现了器件的激子管理并获得了高亮度的白光发射。我们将在以下两个方面开展进一步研究。材料方面,需要找到成膜性更好能级更加匹配的聚合物主体以便可以获得更加优化的磷光敏化荧光。器件制备方面,需要通过器件结构的设计与制备方法的改进来改善器件发光的色稳定性问题。
ABSTRACT: Organic light emitting device (OLED) has been attracting a great deal of attention for its potential to be the next generation technology for lighting and display. However, this theoretical upper limit is only25%of the corresponding quantum efficiency for electroluminescence from the regular OLED, which limits the development of OLED. As phosphorescent materials were presented, it becomes possible to use triplet state to realize high efficient phosphorescence, which provides the possibility to break through the theoretical limit of25%quantum. Although the use of phosphorescent materials can significantly increase the efficiency of OLED, the rolling off of electrophosphorescent efficiency at high current density has been denounced. Some investigate shows that the rolling off of efficiency results from triplet-triplet annihilation at high current density. For sake of finding out the ways to reduce the rolling off of electrophosphorescent efficiency, in this dissertation, phosphorescent material to fluorescent material were codoped the host to reduce the lifetime of triplet state and the triplet-triplet annihilation through the energy transfer from phosphorescent material to fluorescent material. By the way, some tries to realize the high luminance white OLED were made by choosing the appropriate fluorescent dopant which could emit complementary color of phosphorescent dopant and designing a appropriated device structure. We investigated the relative principle for phosphorescent sensitized fluorescence in detail as well. The phosphorescent sensitized OLED provides a ability to enhance the efficiency of OLED for their larger exciton cross section and less triplet lifetime can prevent the triplet-triplet annihilation. The dissertation consists of five chapters. In the first chapter, we summarize the recent progress of White OLED and introduce the relative organic light emitting material, operation principle of device and the method of researching and measuring of OLED. In the other chapters, we present the detail of our research. The detail is listed as below.
In chapter2, we verified the determined effect of the energy transfer from Fir6to rubrene on the emission from PVK:Fir6:rubrene co-dopant OLED by analyzing the absorption spectrum, excited spectrum and steady state photo-luminescence spectrum. We also proved the viability of reducing the efficiency rolling off of electrophosphorescentce at high current density by utilizing Foster energy transfer from Fir6to rubrene to reduce triplet lifetime of Fir6and realized the efficiency enhancement of phosphorescent OLED. Phosphorescent sensitized fluorescent luminescence could be a effective way to enhance the efficiency of phosphorescent OLED at high current density.
In chapter3, we put our attention on the color-shift problem in phosphorescent and fluorescent co-dopants OLED. At first, we exclude that the shift of recombination zone under electric field and saturation of fluorescent co-dopant at high current density result in the color-shift. The electric field enhanced Dexter energy transfer from Fir6to rubrene could be responsible for the color-shift problem by analyzing the electric modulated PL spectrum and transient PL of OLED based on PVK:Fir6:rubrene. As well we found out that carrier trapping effect of rubrene is important for the spectrum-shift as voltage increasing. By avoiding the energy transfer between the two dopants in co-dopants OLED to prevent the color-shift, we realized the white emitting by combing the emission from electromer of TAPC monomer of perylene.
In chapter4, We obtained a high luminance white OLED depending on the structure designing with excitons management, in which green phosphorescent material (Ir(ppy)3) sensitize the red fluorescent material(DCJTB). For the sake of improving the chromaticity dependence of white color on the applied voltage, PVK:Ir(ppy)3:DCJTB (100:5:0.4in wt.) polymer was chosen to combine with NPB blue fluorescent material to obtain the white light emitting. At last, we realized the excitons management and obtained the white OLED with8700cd/m2maximum luminance and41m/w luminous efficiency by controlling the recombination zone utilizing the device structure of ITO/PEDOT:PSS (30nm)/PVK:Ir(ppy)3:DCJTB (100:5:0.4in wt.)(60nm)/NPB(4nm)/BCP(10nm)/Alq3(20nm)/LiF(1nm)/Al(100nm).
In chapter5, We present the conclusions and future work。Upon above research, we could conclude that1, The rolling off of electrophosphorescent efficiency at high current density could be relieved by phosphorescent sensitized fluorescence and efficiency enhancement of OLED could be achieved.2,The color stability could be affected by the electric field enhanced Dexter energy transfer from Fir6to rubrene and carrier trapping effect of rubrene.3, The exciton management and highly luminance white OLED was realized by the structure design of OLED. In my opinion, there are something more to research. The one is to achieve better phosphorescent sensitized fluorescence, the polymer host which have better film-forming and more appropriate energy bandgap was needed. The other one is the research on architecture and fabrication of OLED is needed to improve the color stability of OLED.
引文
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