基于电极界面调控提高有机电致发光器件性能的研究
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摘要
近年来，有机电致发光器件（OLED）以其质量轻、成本低、材料选择丰富、功耗低，尤其是可实现柔性等优点，受到了越来越多的关注。OLED作为平板显示虽然已经在手机等少数电子产品上应用，但距离大规模应用还有较大差距。面向应用，效率和稳定性等性能还需要进一步提升。OLED的性能归根结底是和器件内部功能层的表面界面密切相关的。本论文的工作从电极界面调控的角度展开工作，具体通过实现电极表面的超平滑以及表面的周期性微结构制备等界面形貌调控和对电极进行p型掺杂等界面能带调控，提高了有机电致发光器件的效率、稳定性和视角等。取得的研究成果主要包括以下几个方面：
（1）在柔性衬底上制备了亚纳米量级粗糙度的超平滑银膜，并将其应用到有机电致发光器件当中，得到了高度柔性和高效率的器件。相对于在硅衬底上制备的传统器件，具有超平滑电极的有机电致发光器件效率有60%的提升，这些效率的提升来源于底电极表面粗糙度的降低，形成了接触面积更大的底电极与有机材料界面，使得载流子注入，传输能力获得提高。不仅如此，我们还利用结构化的聚合物封装膜对得到的柔性顶发射器件进行了封装，提高了器件的光取出效率和寿命。并且由于结构化的封装膜表面疏水角大，表面能小，减小了水和灰尘附着造成污染的几率，使得器件具有一定的自清洁特性。
（2）基于超平滑聚合物电极（PEDOT: PSS）的ITO-free柔性OLED。制备了超平滑的聚合物电极（PEDOT: PSS），并应用于柔性OLED，与传统工艺制备的PEDOT:PSS电极相比，其平整度和导电性都有显著提高。器件的效率由传统器件的4.71cd/A提升到了6.21cd/A,提高了38%。为了提升PEDOT: PSS电极的导电性，需用硫酸对PEDOT：PSS进行处理。利用脱模工艺技术，在提高电极表面平整性的同时，可消除硫酸残留对器件稳定性的影响。
（3）石墨烯氧化物掺杂PEDOT: PSS电极，改善电极界面。为了提高PEDOT: PSS电极的性能，对其进行了石墨烯氧化物的p型掺杂。掺杂后电极的空穴注入和电子阻挡能力都有所增强，并且激子的淬灭也得到了抑制。优化后PEDOT: PSS与GO的掺杂比例为15:1，器件的亮度和效率分别由14415cd/m2和3.17cd/A提高到了23871cd/m2和5.71cd/A。
（4）利用周期性微结构电极实现宽光谱白光顶发射OLED。通过将周期性微结构引入顶发射有机电致发光器件中，构建周期性起伏的阳极与有机层界面和相对平坦的阴极与有机界面，解决了白光顶发射有机电致发光器件的光谱窄化和光谱随观察角度蓝移的问题，得到了具有稳定光谱和色坐标的宽光谱白光顶发射OLED。当观察角度从0°变化到60°时，器件的色坐标仅有±0.01的变化。
Organic light-emitting device (OLED) have attracted much attention due to theiradvantages in light weight, low cost, abundant materials, low power consumption, andparticularly, sufficiently ductile of the organic material to undergo significant stresswithout cracking. At present, OLED has been used into a mobile phone and a fewother electronic products. Howerer, it is far away from large scale appilicaton. Theperformances, such as efficiency and lifetime, need to be improved. It is nowappreciated that the electrode/organic functional materials interfaces play animportant role in determining the performance of organic optoelectronic devices. Inthis thesis, much research has been done based on regulation of interface betweenelectrode and organic materials. We have realized the improvement of efficiency,stablility and viewing angle by regulating morphology of interface throughultrasmooth electrode and structured electrode and regulating energy band throughp-doping. The research results include the following aspects:
(1) An ultrasmooth Ag film with sub-nanometer surface roughness on flexiblesubstrate has been fabricated by template stripping process and its effect on organicmaterials deposition and carrier injection and transport in OLEDs has beeninvestigated. We demonstrate highly flexible and efficient OLED which based on theultrasmooth electrode. Compared with conventional devices on Si substrate, theefficiency of devices fabricated with ultrasmooth electrode have60%enhancement. These improvements are obviously originated from carrier injection and transportenhancement as a result of lowered surface roughness of Ag electrode. Moreover, wehave demonstrated a structured polymer encapsulation film on top of TOLED whichcan realize the enhancement of light extraction, the prolongation of lifetime bypreventing moisture and oxygen diffusion into the devices. In addition, theencapsulated devices also have the ability of self-cleaning due to the decrease ofpollution by water droplets and dust arising from high contact angle of structuredsurface.
(2) An efficient ITO-free flexible OLED with ultrasmooth PEDOT: PSS anodehas been demonstrated. The ultrasmooth polymer electrode have been fabricated andapplied to flexible OLED. Compared to spin-coated PEDOT: PSS film on glasssubstrate, the PEDOT: PSS film on polymer substrate fabricated by employingtemplate stripping process has shown superiority on both conductivity and surfacemorphology. The OLED on polymer substrate has also exhibited higher efficiency. Itsmaximum current efficiency is6.21cd/A, while it is4.71cd/A for that with theas-deposited PEDOT: PSS anode on glass substrate, which corresponds to38%enhancement. To further enhance the conduction of PEDOT: PSS film, H2SO4-treatedhas been used. The effect of residual H2SO4on the surface of PEDOT: PSS in H2SO4treatment has been eliminated by template stripping process.
(3) Graphene oxide (GO) has been used as p-dopant into PEDOT: PSS anode toimprove interface between electrode and organic layer. The GO doped into PEDOT:PSS was beneficial to the performance of OLED. The hole-injection ability and electron blocking effect were both improved and the exciton quenching was alsosuppressed. The PEDOT: PSS/GO (15/1) was optimal doping concentration. In caseof this condition, the maximum luminance and efficiency was23871cd/m2and5.71cd/A while they were14415cd/m2and3.67cd/A with undoped PEDOT: PSS anode.
(4) WTOLED with angle-independent broadband emission has beendemonstrated by integrating a periodic microstruture into the device structure toconstruct a cavity with gradually changed cavity length. From building a periodicallycorrugated anode and a relatively planar cathode, the shift of the peak emissionwavelength with the viewing angle is successfully suppressed, and moreover, adesired broad emissive spectrum and stable CIE coordinates are both obtained. Thevariation of the CIE coordinates is within±0.01when the viewing angle changedfrom0°to60°.
（1）在柔性衬底上制备了亚纳米量级粗糙度的超平滑银膜，并将其应用到有机电致发光器件当中，得到了高度柔性和高效率的器件。相对于在硅衬底上制备的传统器件，具有超平滑电极的有机电致发光器件效率有60%的提升，这些效率的提升来源于底电极表面粗糙度的降低，形成了接触面积更大的底电极与有机材料界面，使得载流子注入，传输能力获得提高。不仅如此，我们还利用结构化的聚合物封装膜对得到的柔性顶发射器件进行了封装，提高了器件的光取出效率和寿命。并且由于结构化的封装膜表面疏水角大，表面能小，减小了水和灰尘附着造成污染的几率，使得器件具有一定的自清洁特性。
（2）基于超平滑聚合物电极（PEDOT: PSS）的ITO-free柔性OLED。制备了超平滑的聚合物电极（PEDOT: PSS），并应用于柔性OLED，与传统工艺制备的PEDOT:PSS电极相比，其平整度和导电性都有显著提高。器件的效率由传统器件的4.71cd/A提升到了6.21cd/A,提高了38%。为了提升PEDOT: PSS电极的导电性，需用硫酸对PEDOT：PSS进行处理。利用脱模工艺技术，在提高电极表面平整性的同时，可消除硫酸残留对器件稳定性的影响。
（3）石墨烯氧化物掺杂PEDOT: PSS电极，改善电极界面。为了提高PEDOT: PSS电极的性能，对其进行了石墨烯氧化物的p型掺杂。掺杂后电极的空穴注入和电子阻挡能力都有所增强，并且激子的淬灭也得到了抑制。优化后PEDOT: PSS与GO的掺杂比例为15:1，器件的亮度和效率分别由14415cd/m2和3.17cd/A提高到了23871cd/m2和5.71cd/A。
（4）利用周期性微结构电极实现宽光谱白光顶发射OLED。通过将周期性微结构引入顶发射有机电致发光器件中，构建周期性起伏的阳极与有机层界面和相对平坦的阴极与有机界面，解决了白光顶发射有机电致发光器件的光谱窄化和光谱随观察角度蓝移的问题，得到了具有稳定光谱和色坐标的宽光谱白光顶发射OLED。当观察角度从0°变化到60°时，器件的色坐标仅有±0.01的变化。
Organic light-emitting device (OLED) have attracted much attention due to theiradvantages in light weight, low cost, abundant materials, low power consumption, andparticularly, sufficiently ductile of the organic material to undergo significant stresswithout cracking. At present, OLED has been used into a mobile phone and a fewother electronic products. Howerer, it is far away from large scale appilicaton. Theperformances, such as efficiency and lifetime, need to be improved. It is nowappreciated that the electrode/organic functional materials interfaces play animportant role in determining the performance of organic optoelectronic devices. Inthis thesis, much research has been done based on regulation of interface betweenelectrode and organic materials. We have realized the improvement of efficiency,stablility and viewing angle by regulating morphology of interface throughultrasmooth electrode and structured electrode and regulating energy band throughp-doping. The research results include the following aspects:
(1) An ultrasmooth Ag film with sub-nanometer surface roughness on flexiblesubstrate has been fabricated by template stripping process and its effect on organicmaterials deposition and carrier injection and transport in OLEDs has beeninvestigated. We demonstrate highly flexible and efficient OLED which based on theultrasmooth electrode. Compared with conventional devices on Si substrate, theefficiency of devices fabricated with ultrasmooth electrode have60%enhancement. These improvements are obviously originated from carrier injection and transportenhancement as a result of lowered surface roughness of Ag electrode. Moreover, wehave demonstrated a structured polymer encapsulation film on top of TOLED whichcan realize the enhancement of light extraction, the prolongation of lifetime bypreventing moisture and oxygen diffusion into the devices. In addition, theencapsulated devices also have the ability of self-cleaning due to the decrease ofpollution by water droplets and dust arising from high contact angle of structuredsurface.
(2) An efficient ITO-free flexible OLED with ultrasmooth PEDOT: PSS anodehas been demonstrated. The ultrasmooth polymer electrode have been fabricated andapplied to flexible OLED. Compared to spin-coated PEDOT: PSS film on glasssubstrate, the PEDOT: PSS film on polymer substrate fabricated by employingtemplate stripping process has shown superiority on both conductivity and surfacemorphology. The OLED on polymer substrate has also exhibited higher efficiency. Itsmaximum current efficiency is6.21cd/A, while it is4.71cd/A for that with theas-deposited PEDOT: PSS anode on glass substrate, which corresponds to38%enhancement. To further enhance the conduction of PEDOT: PSS film, H2SO4-treatedhas been used. The effect of residual H2SO4on the surface of PEDOT: PSS in H2SO4treatment has been eliminated by template stripping process.
(3) Graphene oxide (GO) has been used as p-dopant into PEDOT: PSS anode toimprove interface between electrode and organic layer. The GO doped into PEDOT:PSS was beneficial to the performance of OLED. The hole-injection ability and electron blocking effect were both improved and the exciton quenching was alsosuppressed. The PEDOT: PSS/GO (15/1) was optimal doping concentration. In caseof this condition, the maximum luminance and efficiency was23871cd/m2and5.71cd/A while they were14415cd/m2and3.67cd/A with undoped PEDOT: PSS anode.
(4) WTOLED with angle-independent broadband emission has beendemonstrated by integrating a periodic microstruture into the device structure toconstruct a cavity with gradually changed cavity length. From building a periodicallycorrugated anode and a relatively planar cathode, the shift of the peak emissionwavelength with the viewing angle is successfully suppressed, and moreover, adesired broad emissive spectrum and stable CIE coordinates are both obtained. Thevariation of the CIE coordinates is within±0.01when the viewing angle changedfrom0°to60°.
引文
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