基于聚芴为主体材料的高效聚合物电致磷光器件的研究
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摘要
有机发光二极管（OLEDs）分为有机小分子发光二极管（OLED）和聚合物发光二极管（PLED）两种，它们由于在发光、显示、背光源等方面的应用得到了学术界和工业界的广泛关注。虽然小分子的有机发光二极管已经得到了商业化的发展，但是由于设备投资过大，价格过高的原因，它的市场竞争力仍然需要增强。另外一方面，基于聚合物的发光二极管由于可以通过溶液加工工艺，如旋涂、喷墨打印、丝网印刷技术等低成本方法实现，也得到了广泛的关注。即便如此，基于聚合物的发光二极管在效率等方面都需要做进一步的改善。本文主要研究以聚芴（PFO）为主体材料的聚合物电致磷光器件，同时做了一些界面材料对光电子器件性能的影响。
在前人的工作基础上，我们知道聚芴类材料具有较高荧光量子产率和电致发光效率，并且具有深蓝的光谱特性，因此是一种比较理想的主体材料。但是聚芴类材料具有较低的三线态能级，在掺杂磷光三线态材料的时候，如果客体磷光材料的三线态能级高于聚芴的三线态能级时，就会导致能量从客体的三线态能级反转到主体的三线态能级上，从而导致器件的发光淬灭。因此一般来讲，聚芴本身只能作为红光磷光的主体材料，而不能作为绿光和蓝光磷光的主体材料。但是，最近我们发现当在空穴注入层PEDOT：PSS和发光活性层之间插入一层具有高三线态能级的材料PVK作为缓冲层时，我们可以利用聚芴为主体材料获得高效的绿光器件。基于这样的思路，我们通过掺杂FIrpic蓝色磷光材料的方法，做了以PVK为缓冲层，以PFO为主体的高效蓝光器件。随后，我们又做了一些相关的研究，全文工作主要分为以下几个部分。
首先，我们以PVK为空穴缓冲层，把FIrpic掺杂到PFO-POSS主体中实现了高效的蓝光发射，实验证明，当FIrpic的掺杂比例为10%的时候，我们得到了电流效率为16.8cd/A的蓝光发射。为了进一步提高器件效率，我们在PFO-POSS与FIrpic的混合母体中掺杂电子传输材料来提高活性层的电子迁移率。最后，通过掺杂40%的电子传输材料OXD-7，我们获得了电流效率为26.4cd/A，功率效率为17lm/W的高效蓝光器件，并且器件具有较低的启亮电压(3.6V)。和以PVK为主体的蓝光器件相比，我们在效率以及启亮电压方面都存在很多优势。利用器件能级以及激子寿命等方面分析，我们研究了获得高效蓝光器件的原因。
在以聚芴为主体获得高效蓝光器件的基础上，我们通过在蓝光器件中掺杂黄色磷光客体的方法，研究了以PFO-POSS为主体的高效白光器件。通过改变黄光磷光的掺杂比例，我们得到了电流效率为40.9cd/A，功率效率为31.4lm/W的高效白光器件，并且具有较低的启亮电压（3.4V）。随后，我们也研究了以PVK和PFO-POSS为主体的双层发光白光器件，通过将Ir(piq)掺杂到PVK中实现红光发射，FIrpic掺杂到PFO-POSS中实现蓝光发射，我们最终得到了电流效率为12.1cd/A的双层白光器件。
由于有机发光器件为双载流子注入器件，因此有效的载流子注入是获得高效发光器件的基本要素，在这个思路的指导下，我们研究了含硫氧芴（SO）基团的电子注入材料PFN-SO在发光器件中的应用。利用这种电子注入材料，我们研究了其对红绿蓝三色材料的电子注入性能，研究表明，对于这三种不同带隙的材料，PFN-SO皆能够实现高效的电子注入功能，和CsF/Al阴极器件相比，以PFN-SO/Al为阴极的器件能够获得相当的效率，远远高于以Al为单独阴极的器件。研究发现，即便以金属Au为阴极，这种材料也具有较好的电子注入性能。基于上面的结果，我们最后分析了这种材料提高电子注入的原因。
最近，倒置光电子器件由于其潜在的有利因素引起了人们的广泛关注，并且实验也证明，利用水醇溶性的电子注入材料能够显著增强ITO的电子注入功能，获得高效的倒置光电子器件。这里，我们利用电子注入材料PFN-SO也实现了高效的倒置发光器件。通过UPS测试，我们发现，PFN-SO能够降低ITO的功函数，因此能够实现高效的电子注入。
Organic light-emitting diodes (OLEDs) include organic small molecule light-emittingdiode (OLED) and polymer light-emitting diode (PLED), and they have drawn great attentionby academic and industrial sections because of the attractive prospect of application in thelighting, display, backlighting and other fields. Although organic small molecule organiclight-emitting diodes have been commercially developed, due to the expensive equipmentinvestment, the product price is too high, so it sill needs to enhance its marketcompetitiveness. On the other hand, PLED based on polymer can be achieved bysolution-processed, such as spin-coating, inkjet printing and screen printing and otherlow-cost methods, which have drawn widespread attention. However, compared with OLED,PLED still need further improvement in luminous efficiency and other areas. In this article,we will mainly use the polyfluorene (PFO) as the host to improve the luminous efficiency ofPLED; besides, the effection of interface materials on the performance of optoelectronicdevices are also included.
On the basis of previous work, we know that the polyfluorene and its dericatives havehigh fluorescence quantum efficiency, high electroluminescent efficiency anddeep-blue-emitting properties; therefore, it’s an ideal host material. But polyfluorene and itsdericatives have lower-lying triplet energy levels, so when the phosphorescent materials aredoped into the PFO host, if the triplet energy levels of the phosphorescent materials werehigher than PFO host, it would cause energy back transfer and could not get efficientlight-emitting. Therefore, the PFO itself is often used as the host for the red phosphorescentmaterials, but can not be used as the host for the green and blue phosphorescent materials.Recently, we find that if we insert a PVK layer which has a higher-lying triplet energy levelsbetween the PEDOT: PSS and the emitting layer as a buffer layer, we can get efficient greenphosphorescence emission by using the PFO as the host. Based on this idea, we get efficientblue light by doping the blue phosphorescent material FIrpic into the PFO host as theemitting layer and PVK as the buffer layer. Other researches about PLED are also included inthis article. The work is mainly divided into the following parts.
In the first part, we get efficient blue light by doping the FIrpic into the PFO-POSS host, PVK as the buffer layer. Experiment shows that when the proportion of FIrpic is10%, we getefficient blue light with the luminous efficiency of16.8cd/A. In order to further improve thedevice efficiency, we dope electron transport material (OXD-7) into the PFO-POSS: FIrpichost. When the proportion of OXD-7is40%, we get efficient blue light with the luminousefficiency of26.4cd/A, power efficiency of17lm/W and a low turn on voltage (3.6V).Compared with the blue device using the PVK as the host, this device has higher efficiencyand lower turn-on voltage. Finally, we discuss the reasons why we get so high deviceefficiency by energy levels and exciton lifetime of this device.
Based on the efficient blue light devices that we get in the first part, in this part, westudy the white light-emitting devices based on the PFO-POSS as the host by doping anorange phosphorescent material into the blue devices. By changing the doping proportion oforganic phosphorescent material, we get efficient white light with the luminous efficiency of40.9cd/A, power efficiency of31.4lm/W and a low turn on voltage (3.4V). Then, we studythe efficient white-light-emitting diodes based on bilayer structure. By doping the Ir(piq) intothe PVK host to emitting red light, FIrpic into the PFO-POSS host to emitting blue light, wefinally get efficient white light with a luminous efficiency of12.1cd/A with this bilayerstructure.
As we know, efficient charge injection and transport are a basic requirement for highlyefficient light-emitting devices. Under the guidance of this idea, we study the character of anelectron injection material containing SO group in the light-emitting devices. By using thiselectron injection material PFN-SO as the electron injection layer and three different polymermaterials as the emitting layer, we find that the electron injection material PFN-SO canimprove the electron injection efficiently. Compared with the devices using CsF/Al as thecathode, the devices using PFN-SO/Al as the cathode can get similar results, far higher thanthe results using Al only as the cathode. We also find that this electron injection material haveefficient electron injection character even if we use the metal Au as the cathode. At last, weanalyze the reasons why this material can improve the electron injection efficiently.
Recently, inverted devices have drawn a lot of attention because of its potentialadvantages. On the other hand, a variety of electron-injection conjugated polyelectrolyte,especially water/alcohol soluble polyfluorenes, have been reported to be able to realize efficient electron injection using ITO as the cathode and get efficient inverted devices. Here,we get efficient inverted light-emitting device with ITO/PFN-SO as the cathode andMoO3/Al as the anode. From the UPS analyze, we find that the PFN-SO layer can lower thework function of ITO, so it can inject electron efficiently.
在前人的工作基础上，我们知道聚芴类材料具有较高荧光量子产率和电致发光效率，并且具有深蓝的光谱特性，因此是一种比较理想的主体材料。但是聚芴类材料具有较低的三线态能级，在掺杂磷光三线态材料的时候，如果客体磷光材料的三线态能级高于聚芴的三线态能级时，就会导致能量从客体的三线态能级反转到主体的三线态能级上，从而导致器件的发光淬灭。因此一般来讲，聚芴本身只能作为红光磷光的主体材料，而不能作为绿光和蓝光磷光的主体材料。但是，最近我们发现当在空穴注入层PEDOT：PSS和发光活性层之间插入一层具有高三线态能级的材料PVK作为缓冲层时，我们可以利用聚芴为主体材料获得高效的绿光器件。基于这样的思路，我们通过掺杂FIrpic蓝色磷光材料的方法，做了以PVK为缓冲层，以PFO为主体的高效蓝光器件。随后，我们又做了一些相关的研究，全文工作主要分为以下几个部分。
首先，我们以PVK为空穴缓冲层，把FIrpic掺杂到PFO-POSS主体中实现了高效的蓝光发射，实验证明，当FIrpic的掺杂比例为10%的时候，我们得到了电流效率为16.8cd/A的蓝光发射。为了进一步提高器件效率，我们在PFO-POSS与FIrpic的混合母体中掺杂电子传输材料来提高活性层的电子迁移率。最后，通过掺杂40%的电子传输材料OXD-7，我们获得了电流效率为26.4cd/A，功率效率为17lm/W的高效蓝光器件，并且器件具有较低的启亮电压(3.6V)。和以PVK为主体的蓝光器件相比，我们在效率以及启亮电压方面都存在很多优势。利用器件能级以及激子寿命等方面分析，我们研究了获得高效蓝光器件的原因。
在以聚芴为主体获得高效蓝光器件的基础上，我们通过在蓝光器件中掺杂黄色磷光客体的方法，研究了以PFO-POSS为主体的高效白光器件。通过改变黄光磷光的掺杂比例，我们得到了电流效率为40.9cd/A，功率效率为31.4lm/W的高效白光器件，并且具有较低的启亮电压（3.4V）。随后，我们也研究了以PVK和PFO-POSS为主体的双层发光白光器件，通过将Ir(piq)掺杂到PVK中实现红光发射，FIrpic掺杂到PFO-POSS中实现蓝光发射，我们最终得到了电流效率为12.1cd/A的双层白光器件。
由于有机发光器件为双载流子注入器件，因此有效的载流子注入是获得高效发光器件的基本要素，在这个思路的指导下，我们研究了含硫氧芴（SO）基团的电子注入材料PFN-SO在发光器件中的应用。利用这种电子注入材料，我们研究了其对红绿蓝三色材料的电子注入性能，研究表明，对于这三种不同带隙的材料，PFN-SO皆能够实现高效的电子注入功能，和CsF/Al阴极器件相比，以PFN-SO/Al为阴极的器件能够获得相当的效率，远远高于以Al为单独阴极的器件。研究发现，即便以金属Au为阴极，这种材料也具有较好的电子注入性能。基于上面的结果，我们最后分析了这种材料提高电子注入的原因。
最近，倒置光电子器件由于其潜在的有利因素引起了人们的广泛关注，并且实验也证明，利用水醇溶性的电子注入材料能够显著增强ITO的电子注入功能，获得高效的倒置光电子器件。这里，我们利用电子注入材料PFN-SO也实现了高效的倒置发光器件。通过UPS测试，我们发现，PFN-SO能够降低ITO的功函数，因此能够实现高效的电子注入。
Organic light-emitting diodes (OLEDs) include organic small molecule light-emittingdiode (OLED) and polymer light-emitting diode (PLED), and they have drawn great attentionby academic and industrial sections because of the attractive prospect of application in thelighting, display, backlighting and other fields. Although organic small molecule organiclight-emitting diodes have been commercially developed, due to the expensive equipmentinvestment, the product price is too high, so it sill needs to enhance its marketcompetitiveness. On the other hand, PLED based on polymer can be achieved bysolution-processed, such as spin-coating, inkjet printing and screen printing and otherlow-cost methods, which have drawn widespread attention. However, compared with OLED,PLED still need further improvement in luminous efficiency and other areas. In this article,we will mainly use the polyfluorene (PFO) as the host to improve the luminous efficiency ofPLED; besides, the effection of interface materials on the performance of optoelectronicdevices are also included.
On the basis of previous work, we know that the polyfluorene and its dericatives havehigh fluorescence quantum efficiency, high electroluminescent efficiency anddeep-blue-emitting properties; therefore, it’s an ideal host material. But polyfluorene and itsdericatives have lower-lying triplet energy levels, so when the phosphorescent materials aredoped into the PFO host, if the triplet energy levels of the phosphorescent materials werehigher than PFO host, it would cause energy back transfer and could not get efficientlight-emitting. Therefore, the PFO itself is often used as the host for the red phosphorescentmaterials, but can not be used as the host for the green and blue phosphorescent materials.Recently, we find that if we insert a PVK layer which has a higher-lying triplet energy levelsbetween the PEDOT: PSS and the emitting layer as a buffer layer, we can get efficient greenphosphorescence emission by using the PFO as the host. Based on this idea, we get efficientblue light by doping the blue phosphorescent material FIrpic into the PFO host as theemitting layer and PVK as the buffer layer. Other researches about PLED are also included inthis article. The work is mainly divided into the following parts.
In the first part, we get efficient blue light by doping the FIrpic into the PFO-POSS host, PVK as the buffer layer. Experiment shows that when the proportion of FIrpic is10%, we getefficient blue light with the luminous efficiency of16.8cd/A. In order to further improve thedevice efficiency, we dope electron transport material (OXD-7) into the PFO-POSS: FIrpichost. When the proportion of OXD-7is40%, we get efficient blue light with the luminousefficiency of26.4cd/A, power efficiency of17lm/W and a low turn on voltage (3.6V).Compared with the blue device using the PVK as the host, this device has higher efficiencyand lower turn-on voltage. Finally, we discuss the reasons why we get so high deviceefficiency by energy levels and exciton lifetime of this device.
Based on the efficient blue light devices that we get in the first part, in this part, westudy the white light-emitting devices based on the PFO-POSS as the host by doping anorange phosphorescent material into the blue devices. By changing the doping proportion oforganic phosphorescent material, we get efficient white light with the luminous efficiency of40.9cd/A, power efficiency of31.4lm/W and a low turn on voltage (3.4V). Then, we studythe efficient white-light-emitting diodes based on bilayer structure. By doping the Ir(piq) intothe PVK host to emitting red light, FIrpic into the PFO-POSS host to emitting blue light, wefinally get efficient white light with a luminous efficiency of12.1cd/A with this bilayerstructure.
As we know, efficient charge injection and transport are a basic requirement for highlyefficient light-emitting devices. Under the guidance of this idea, we study the character of anelectron injection material containing SO group in the light-emitting devices. By using thiselectron injection material PFN-SO as the electron injection layer and three different polymermaterials as the emitting layer, we find that the electron injection material PFN-SO canimprove the electron injection efficiently. Compared with the devices using CsF/Al as thecathode, the devices using PFN-SO/Al as the cathode can get similar results, far higher thanthe results using Al only as the cathode. We also find that this electron injection material haveefficient electron injection character even if we use the metal Au as the cathode. At last, weanalyze the reasons why this material can improve the electron injection efficiently.
Recently, inverted devices have drawn a lot of attention because of its potentialadvantages. On the other hand, a variety of electron-injection conjugated polyelectrolyte,especially water/alcohol soluble polyfluorenes, have been reported to be able to realize efficient electron injection using ITO as the cathode and get efficient inverted devices. Here,we get efficient inverted light-emitting device with ITO/PFN-SO as the cathode andMoO3/Al as the anode. From the UPS analyze, we find that the PFN-SO layer can lower thework function of ITO, so it can inject electron efficiently.
引文
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