有机电致发光器件的载流子调控与性能研究
发布时间：2018-07-13 16:09
【摘要】：有机电致发光器件(organic light-emitting diodes,OLEDs),具有材料来源广、全固态主动发光、效率高、柔性超薄、大面积和多功能应用等优点,迅速成为信息显示领域的技术热点,正在逐步实现大规模的商业化生产。近些年,随着新的材料、结构和工艺的快速发展以及发光机理的深入研究,OLEDs基础研究和应用技术取得了巨大的进步。然而目前OLEDs仍然存在着器件效率、稳定性、良品率和成本等方面的问题,需要继续以基础研究为突破点,在器件结构设计和优化上开展工作,深入研究器件内部载流子调控对器件性能的影响。针对上述OLEDs中存在的问题,本文采用载流子调控方法改善双发光层OLEDs内载流子的平衡;采用具有双极特性的荧光材料作为载流子调控和发光层制备白光有机电致发光器件(WOLEDs);研究有机体异质结电荷产生层对提高串联OLEDs器件性能的作用机理;将载流子调控运用到倒置型聚合物太阳能电池(Inverted polymer solar cells,IPSCs)中,制备基于ZnO阴极修饰层的高性能器件。同时,分析讨论载流子调控的机理,研究载流子调控结构对器件性能的影响,以此促进OLEDs的商业化应用进程。主要的研究内容包括:1、研究载流子调控结构对磷光OLEDs器件性能的影响及作用机理采用空穴传输材料N,N′-bis(naphthalen-1-yl)-N,N′-bis(phenyl)-benzidine(NPB)作为空穴传输层和第一发光层主体,双极性材料4,4’-bis(carbazol-9-yl)biphenyl(CBP)作为第二发光层主体,橙色磷光染料bis[2-(4-tert-butylphenyl)-benzothiazolato-N,C2]iridium(acetylacetonate)(t-bt)2Ir(acac)作为客体,制备具有双发光层结构的磷光OLEDs(phosphorescent OLEDs,PhOLEDs),讨论载流子调控结构对载流子平衡和载流子复合区域拓展的影响及作用机制。研究发现,采用优化的双发光层器件的启亮电压是3.3 V,最大发光亮度为30898 cd/m2,相比单发光层器件,启亮电压降低了36.5%,亮度增加了174%。同时,双发光层器件的功率效率显著提升,效率滚降得到了明显的抑制。载流子调控结构的主要作用是消除空穴传输层到第一发光层主体的最高占有分子轨道(highest occupied molecular orbital,HOMO)能级势垒被消除,减少界面载流子的累积;增加电子和空穴的传输通道,实现了器件内载流子的平衡;拓展载流子复合区域,提高了载流子的利用率,实现高效发光和提升器件稳定性。同时,实验采用具有不同载流子传输能力的间隔层Alq3、TAPC、CBP和mCP分别制备了白光PhOLEDs,并研究了间隔层对器件性能的影响以及对器件内载流子输运和能量转移的作用机制。研究发现基于Alq3间隔层的器件获得了最低的启亮电压6.2v,最优的白光cie色坐标(0.35,0.34)。2、研究载流子调控结构对woleds器件性能和光谱特性的影响采用双极性绿色荧光材料2-{4-[bis(9,9-dimethylfluorenyl)amino]plenyl}-5-(dimesitylboryl)thiophene(flamb-1t)作为载流子调控层和绿色发光层,结合3-(dicyanomethylene)-5,5-dimethyl-1-(4-dimethylamino-styryl)cyclohexene(dcddc)红光超薄层和4,4′-bis(2,2′-diphenyvinyl)-1,1′-dipenyl(dpvbi)蓝光层,制备了非掺杂的三原色woleds,讨论了flamb-1t双极性发光层的厚度对器件性能和载流子复合核心区域的影响。研究发现,flamb-1t厚度从3nm增加到15nm时,器件亮度和最大功率效率显著提升218%和330%。f1amb-1t载流子调控层的主要作用是通过其电子和空穴的双极传输特性,有效的实现白光器件内的载流子传输平衡;构建flamb-1t/dcddc/flamb-1t载流子陷阱结构,采用直接载流子捕获的方式实现dcddc红光发射,从而调控载流子的复合中心,实现白光发射。当flamb-1t为10nm时,获得commissioninternationaledel'eclairage(cie)坐标为(0.33,0.36)的woleds。不同电压驱动下,最优化的woleds载流子复合中心位置始终被限制在三个稳定的区域,这说明flamb-1t载流子调控层可以有效的控制激子形成区域。3、研究有机电荷产生层的性能对串联oleds性能的影响采用boronsubphthalocyaninechloride(subpc):fullerene(c60)和cobalt(ii)phthalocyanine(copc):c60两种有机体异质结电荷产生层,分别制备了高性能的串联oleds,研究了电荷产生层载流子调控能力的优化对串联器件性能的影响。研究发现,电荷产生层的优化可以改善有机体异质结界面,增加界面偶极子数量,提升电荷产生层的电荷产生能力;增加载流子传输通道,提升电荷产生层的载流子传输能力,促进器件内载流子的平衡传输,从而改善器件的性能。通过上述研究,优化电荷产生层中给体subpc和copc的含量,获得了最大电流效率分别为63.6cd/a和50.2cd/a串联oleds。4、研究低温热退火zno阴极修饰层对倒置型pscs性能的影响采用低温热退火工艺制备氧化锌(zincoxide,zno)阴极修饰层,研究zno的光电特性对ipscs载流子调控和器件性能的影响。研究发现,真空动态退火工艺可以改善zno薄膜的表面形貌,显著降低的薄膜表面粗糙度这主要归因于热流的分布情况、溶剂的挥发过程和zno前驱体的热分解过程。采用真空动态退火zno的倒置型器件的能量转换效率(power-conversionefficiency,pce)为4.01%,相比原位退火zno的器件性能提升了15.8%,。真空动态退火zno的作用是降低ito/活性层之间的接触电阻,抑制漏电流的产生;同时有效控制器件内载流子的复合过程,提升电子的传输和收集能力,从而改善器件的性能。综上所述,本研究工作设计了具有载流子调控能力的若干种不同结构的OLEDs,为实现高性能的器件奠定了理论基础和提供了理论指导。同时,具有载流子调控能力的Zn O功能层可以用来改善IPSC的器件性能。这表明载流子调控是实现高性能有机光电子器件的有效途径。
[Abstract]:Organic light-emitting diodes (OLEDs), which has the advantages of wide material source, full solid state active luminescence, high efficiency, flexible and thin, large area and multi-functional applications, has become a hot spot in the field of information display, and is gradually realizing large-scale commercial production. In recent years, with new materials, structure and work The rapid development of art and the in-depth study of the mechanism of luminescence have made great progress in the basic research and application technology of OLEDs. However, there are still problems in OLEDs, such as device efficiency, stability, good product rate and cost. It is necessary to continue the basic research as a breakthrough, work on the design and optimization of the device structure and study in depth. In order to solve the problems in the OLEDs, the carrier control method is used to improve the balance of the carrier in the dual luminescent layer OLEDs. The fluorescent material with bipolar characteristics is used as the carrier regulation and the luminescent layer to prepare the white light organic electroluminescent device (WOLEDs), and the organism is studied. The mechanism of heterojunction charge production layer on improving the performance of series OLEDs devices; using carrier regulation in inverted polymer solar cells (Inverted polymer solar cells, IPSCs) to prepare high performance devices based on ZnO cathode modification layer. At the same time, the mechanism of current carrier regulation is discussed and the carrier regulation structure pair is studied. In order to promote the commercial application process of OLEDs, the main research contents include: 1, the study of the effect of carrier control structure on the performance of phosphorescent OLEDs devices and the mechanism of action are cavity transmission materials N, N '-bis (naphthalen-1-yl) -N, N' -bis (phenyl) -benzidine (phenyl) -benzidine (NPB) as the hole transport layer and the first luminescent layer body, The bipolar material 4,4 '-bis (carbazol-9-yl) biphenyl (CBP) is used as the main body of the second luminescent layer, the orange phosphorescent dye bis[2- (4-tert-butylphenyl) -benzothiazolato-N, C2]iridium (acetylacetonate) (t-bt) 2Ir (t-bt) as the object. The influence and mechanism of the carrier balance and carrier complex region expansion are constructed. The study shows that the bright voltage of the optimized double layer device is 3.3 V and the maximum luminance is 30898 cd/m2. Compared with the single luminescent layer, the bright voltage is reduced by 36.5%, the brightness is increased by 174%., and the power efficiency of the dual luminescent layer is remarkable. The main function of the carrier control structure is to eliminate the highest occupant molecular orbital (highest occupied molecular orbital, HOMO) to eliminate the energy level barrier of the first luminescent layer, to reduce the accumulation of the interface carrier, and to increase the transmission channel of the electron and hole, and realize the realization of the device. The carrier is balanced, the carrier recombination area is expanded, the utilization of the carrier is improved, the high efficiency luminescence and the stability of the device are achieved. At the same time, the white light PhOLEDs is prepared by the spacer Alq3, TAPC, CBP and mCP with different carrier transmission capacity, and the influence of the interlayer on the performance of the device and the device are also studied. The mechanism of internal carrier transport and energy transfer. It is found that the lowest bright voltage 6.2V and the optimal white light CIE color coordinate (0.35,0.34).2 are obtained based on the Alq3 interlayer, and the effects of the carrier regulation structure on the performance and spectral properties of WOLEDs devices are used for the dual polar green fluorescent material 2-{4-[bis (9,9-dimethylfluoren). YL) amino]plenyl}-5- (dimesitylboryl) thiophene (flamb-1t) is used as a carrier control layer and a green luminescent layer, combined with a 3- (dicyanomethylene) -5,5-dimethyl-1- (4-dimethylamino-styryl) cyclohexene (dcddc) red light layer and a 4,4 '. The influence of the thickness of the flamb-1t bipolar luminescent layer on the performance of the device and the carrier complex core region is discussed. It is found that when the thickness of the flamb-1t increases from 3nm to 15nm, the device brightness and maximum power efficiency are significantly increased by 218% and the main function of the 330%.f1amb-1t carrier is through the bipolar transmission characteristics of the electrons and holes. It realizes the carrier transmission balance in the white light device, constructs the flamb-1t/dcddc/flamb-1t carrier trap structure and uses the direct carrier capture to realize the dcddc red light emission, thus regulating the complex center of the carrier and realizing the white light emission. When the flamb-1t is 10nm, the commissioninternationaledel'eclairage (CIE) coordinates are obtained. Under the different voltage of woleds. 0.33,0.36, the optimal WOLEDs carrier complex center position is always restricted to three stable regions, which indicates that the flamb-1t carrier control layer can effectively control the.3 of the exciton formation region, and study the effect of the performance of the organic charge generation layer on the performance of the serial OLEDs by boronsubphthalocyaninech Loride (subpc): fullerene (C60) and cobalt (II) phthalocyanine (COPC): C60 two kinds of organism heterojunction charge generation layer, respectively, to prepare high performance series OLEDs respectively. The effect of charge production layer carrier optimization on the performance of series devices is studied. The study shows that the optimization of charge generation layer can improve the heterogeneous boundary of the organism. Surface dipoles increase the number of dipoles, increase the charge generation capacity of the charge generation layer, increase the carrier transmission channel, enhance the carrier transport capacity of the charge generation layer, promote the balanced transmission of the carrier in the device, and improve the performance of the device. Through the above study, the content of the donor subpc and COPC in the charge generation layer is obtained. The maximum current efficiency is 63.6cd/a and 50.2cd/a series oleds.4 respectively. The influence of ZnO cathode modification layer on the properties of inverted PSCs is studied by low temperature annealing process, the effect of the cathode modification layer of Zinc Oxide (zincoxide, ZnO) is prepared by low temperature annealing process. The effect of the photoelectric properties of ZnO on the control of iPSCs carrier and the performance of the device is studied. The surface morphology of ZnO films can be improved by annealing process, which is mainly attributed to the distribution of heat flow, the volatilization process of solvent and the thermal decomposition process of the ZnO precursor. The energy conversion efficiency (power-conversionefficiency, PCE) of the inverted device using vacuum dynamic annealing ZnO is 4.01%, compared to the original. The performance of the bit annealed ZnO has been improved by 15.8%. The function of the vacuum dynamic annealing ZnO is to reduce the contact resistance between the ito/ active layers and suppress the leakage current. At the same time, the complex process of the carrier in the controller parts is used to improve the transmission and collection of the electrons, thus improving the performance of the device. Several different structures of OLEDs with carrier control ability provide theoretical basis and theoretical guidance for the realization of high performance devices. At the same time, the Zn O functional layer with carrier control ability can be used to improve the performance of IPSC devices. This indicates that carrier control is an effective way to realize high performance organic optoelectronic devices.
【学位授予单位】：电子科技大学
【学位级别】：博士
【学位授予年份】：2016
【分类号】：TN383.1
本文编号：2119993
[Abstract]:Organic light-emitting diodes (OLEDs), which has the advantages of wide material source, full solid state active luminescence, high efficiency, flexible and thin, large area and multi-functional applications, has become a hot spot in the field of information display, and is gradually realizing large-scale commercial production. In recent years, with new materials, structure and work The rapid development of art and the in-depth study of the mechanism of luminescence have made great progress in the basic research and application technology of OLEDs. However, there are still problems in OLEDs, such as device efficiency, stability, good product rate and cost. It is necessary to continue the basic research as a breakthrough, work on the design and optimization of the device structure and study in depth. In order to solve the problems in the OLEDs, the carrier control method is used to improve the balance of the carrier in the dual luminescent layer OLEDs. The fluorescent material with bipolar characteristics is used as the carrier regulation and the luminescent layer to prepare the white light organic electroluminescent device (WOLEDs), and the organism is studied. The mechanism of heterojunction charge production layer on improving the performance of series OLEDs devices; using carrier regulation in inverted polymer solar cells (Inverted polymer solar cells, IPSCs) to prepare high performance devices based on ZnO cathode modification layer. At the same time, the mechanism of current carrier regulation is discussed and the carrier regulation structure pair is studied. In order to promote the commercial application process of OLEDs, the main research contents include: 1, the study of the effect of carrier control structure on the performance of phosphorescent OLEDs devices and the mechanism of action are cavity transmission materials N, N '-bis (naphthalen-1-yl) -N, N' -bis (phenyl) -benzidine (phenyl) -benzidine (NPB) as the hole transport layer and the first luminescent layer body, The bipolar material 4,4 '-bis (carbazol-9-yl) biphenyl (CBP) is used as the main body of the second luminescent layer, the orange phosphorescent dye bis[2- (4-tert-butylphenyl) -benzothiazolato-N, C2]iridium (acetylacetonate) (t-bt) 2Ir (t-bt) as the object. The influence and mechanism of the carrier balance and carrier complex region expansion are constructed. The study shows that the bright voltage of the optimized double layer device is 3.3 V and the maximum luminance is 30898 cd/m2. Compared with the single luminescent layer, the bright voltage is reduced by 36.5%, the brightness is increased by 174%., and the power efficiency of the dual luminescent layer is remarkable. The main function of the carrier control structure is to eliminate the highest occupant molecular orbital (highest occupied molecular orbital, HOMO) to eliminate the energy level barrier of the first luminescent layer, to reduce the accumulation of the interface carrier, and to increase the transmission channel of the electron and hole, and realize the realization of the device. The carrier is balanced, the carrier recombination area is expanded, the utilization of the carrier is improved, the high efficiency luminescence and the stability of the device are achieved. At the same time, the white light PhOLEDs is prepared by the spacer Alq3, TAPC, CBP and mCP with different carrier transmission capacity, and the influence of the interlayer on the performance of the device and the device are also studied. The mechanism of internal carrier transport and energy transfer. It is found that the lowest bright voltage 6.2V and the optimal white light CIE color coordinate (0.35,0.34).2 are obtained based on the Alq3 interlayer, and the effects of the carrier regulation structure on the performance and spectral properties of WOLEDs devices are used for the dual polar green fluorescent material 2-{4-[bis (9,9-dimethylfluoren). YL) amino]plenyl}-5- (dimesitylboryl) thiophene (flamb-1t) is used as a carrier control layer and a green luminescent layer, combined with a 3- (dicyanomethylene) -5,5-dimethyl-1- (4-dimethylamino-styryl) cyclohexene (dcddc) red light layer and a 4,4 '. The influence of the thickness of the flamb-1t bipolar luminescent layer on the performance of the device and the carrier complex core region is discussed. It is found that when the thickness of the flamb-1t increases from 3nm to 15nm, the device brightness and maximum power efficiency are significantly increased by 218% and the main function of the 330%.f1amb-1t carrier is through the bipolar transmission characteristics of the electrons and holes. It realizes the carrier transmission balance in the white light device, constructs the flamb-1t/dcddc/flamb-1t carrier trap structure and uses the direct carrier capture to realize the dcddc red light emission, thus regulating the complex center of the carrier and realizing the white light emission. When the flamb-1t is 10nm, the commissioninternationaledel'eclairage (CIE) coordinates are obtained. Under the different voltage of woleds. 0.33,0.36, the optimal WOLEDs carrier complex center position is always restricted to three stable regions, which indicates that the flamb-1t carrier control layer can effectively control the.3 of the exciton formation region, and study the effect of the performance of the organic charge generation layer on the performance of the serial OLEDs by boronsubphthalocyaninech Loride (subpc): fullerene (C60) and cobalt (II) phthalocyanine (COPC): C60 two kinds of organism heterojunction charge generation layer, respectively, to prepare high performance series OLEDs respectively. The effect of charge production layer carrier optimization on the performance of series devices is studied. The study shows that the optimization of charge generation layer can improve the heterogeneous boundary of the organism. Surface dipoles increase the number of dipoles, increase the charge generation capacity of the charge generation layer, increase the carrier transmission channel, enhance the carrier transport capacity of the charge generation layer, promote the balanced transmission of the carrier in the device, and improve the performance of the device. Through the above study, the content of the donor subpc and COPC in the charge generation layer is obtained. The maximum current efficiency is 63.6cd/a and 50.2cd/a series oleds.4 respectively. The influence of ZnO cathode modification layer on the properties of inverted PSCs is studied by low temperature annealing process, the effect of the cathode modification layer of Zinc Oxide (zincoxide, ZnO) is prepared by low temperature annealing process. The effect of the photoelectric properties of ZnO on the control of iPSCs carrier and the performance of the device is studied. The surface morphology of ZnO films can be improved by annealing process, which is mainly attributed to the distribution of heat flow, the volatilization process of solvent and the thermal decomposition process of the ZnO precursor. The energy conversion efficiency (power-conversionefficiency, PCE) of the inverted device using vacuum dynamic annealing ZnO is 4.01%, compared to the original. The performance of the bit annealed ZnO has been improved by 15.8%. The function of the vacuum dynamic annealing ZnO is to reduce the contact resistance between the ito/ active layers and suppress the leakage current. At the same time, the complex process of the carrier in the controller parts is used to improve the transmission and collection of the electrons, thus improving the performance of the device. Several different structures of OLEDs with carrier control ability provide theoretical basis and theoretical guidance for the realization of high performance devices. At the same time, the Zn O functional layer with carrier control ability can be used to improve the performance of IPSC devices. This indicates that carrier control is an effective way to realize high performance organic optoelectronic devices.
【学位授予单位】：电子科技大学
【学位级别】：博士
【学位授予年份】：2016
【分类号】：TN383.1
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