發(fā)布時(shí)間：2018-07-13 16:09

【摘要】：有機(jī)電致發(fā)光器件(organic light-emitting diodes,OLEDs),具有材料來源廣、全固態(tài)主動(dòng)發(fā)光、效率高、柔性超薄、大面積和多功能應(yīng)用等優(yōu)點(diǎn),迅速成為信息顯示領(lǐng)域的技術(shù)熱點(diǎn),正在逐步實(shí)現(xiàn)大規(guī)模的商業(yè)化生產(chǎn)。近些年,隨著新的材料、結(jié)構(gòu)和工藝的快速發(fā)展以及發(fā)光機(jī)理的深入研究,OLEDs基礎(chǔ)研究和應(yīng)用技術(shù)取得了巨大的進(jìn)步。然而目前OLEDs仍然存在著器件效率、穩(wěn)定性、良品率和成本等方面的問題,需要繼續(xù)以基礎(chǔ)研究為突破點(diǎn),在器件結(jié)構(gòu)設(shè)計(jì)和優(yōu)化上開展工作,深入研究器件內(nèi)部載流子調(diào)控對(duì)器件性能的影響。針對(duì)上述OLEDs中存在的問題,本文采用載流子調(diào)控方法改善雙發(fā)光層OLEDs內(nèi)載流子的平衡;采用具有雙極特性的熒光材料作為載流子調(diào)控和發(fā)光層制備白光有機(jī)電致發(fā)光器件(WOLEDs);研究有機(jī)體異質(zhì)結(jié)電荷產(chǎn)生層對(duì)提高串聯(lián)OLEDs器件性能的作用機(jī)理;將載流子調(diào)控運(yùn)用到倒置型聚合物太陽能電池(Inverted polymer solar cells,IPSCs)中,制備基于ZnO陰極修飾層的高性能器件。同時(shí),分析討論載流子調(diào)控的機(jī)理,研究載流子調(diào)控結(jié)構(gòu)對(duì)器件性能的影響,以此促進(jìn)OLEDs的商業(yè)化應(yīng)用進(jìn)程。主要的研究?jī)?nèi)容包括:1、研究載流子調(diào)控結(jié)構(gòu)對(duì)磷光OLEDs器件性能的影響及作用機(jī)理采用空穴傳輸材料N,N′-bis(naphthalen-1-yl)-N,N′-bis(phenyl)-benzidine(NPB)作為空穴傳輸層和第一發(fā)光層主體,雙極性材料4,4’-bis(carbazol-9-yl)biphenyl(CBP)作為第二發(fā)光層主體,橙色磷光染料bis[2-(4-tert-butylphenyl)-benzothiazolato-N,C2]iridium(acetylacetonate)(t-bt)2Ir(acac)作為客體,制備具有雙發(fā)光層結(jié)構(gòu)的磷光OLEDs(phosphorescent OLEDs,PhOLEDs),討論載流子調(diào)控結(jié)構(gòu)對(duì)載流子平衡和載流子復(fù)合區(qū)域拓展的影響及作用機(jī)制。研究發(fā)現(xiàn),采用優(yōu)化的雙發(fā)光層器件的啟亮電壓是3.3 V,最大發(fā)光亮度為30898 cd/m2,相比單發(fā)光層器件,啟亮電壓降低了36.5%,亮度增加了174%。同時(shí),雙發(fā)光層器件的功率效率顯著提升,效率滾降得到了明顯的抑制。載流子調(diào)控結(jié)構(gòu)的主要作用是消除空穴傳輸層到第一發(fā)光層主體的最高占有分子軌道(highest occupied molecular orbital,HOMO)能級(jí)勢(shì)壘被消除,減少界面載流子的累積;增加電子和空穴的傳輸通道,實(shí)現(xiàn)了器件內(nèi)載流子的平衡;拓展載流子復(fù)合區(qū)域,提高了載流子的利用率,實(shí)現(xiàn)高效發(fā)光和提升器件穩(wěn)定性。同時(shí),實(shí)驗(yàn)采用具有不同載流子傳輸能力的間隔層Alq3、TAPC、CBP和mCP分別制備了白光PhOLEDs,并研究了間隔層對(duì)器件性能的影響以及對(duì)器件內(nèi)載流子輸運(yùn)和能量轉(zhuǎn)移的作用機(jī)制。研究發(fā)現(xiàn)基于Alq3間隔層的器件獲得了最低的啟亮電壓6.2v,最優(yōu)的白光cie色坐標(biāo)(0.35,0.34)。2、研究載流子調(diào)控結(jié)構(gòu)對(duì)woleds器件性能和光譜特性的影響采用雙極性綠色熒光材料2-{4-[bis(9,9-dimethylfluorenyl)amino]plenyl}-5-(dimesitylboryl)thiophene(flamb-1t)作為載流子調(diào)控層和綠色發(fā)光層,結(jié)合3-(dicyanomethylene)-5,5-dimethyl-1-(4-dimethylamino-styryl)cyclohexene(dcddc)紅光超薄層和4,4′-bis(2,2′-diphenyvinyl)-1,1′-dipenyl(dpvbi)藍(lán)光層,制備了非摻雜的三原色woleds,討論了flamb-1t雙極性發(fā)光層的厚度對(duì)器件性能和載流子復(fù)合核心區(qū)域的影響。研究發(fā)現(xiàn),flamb-1t厚度從3nm增加到15nm時(shí),器件亮度和最大功率效率顯著提升218%和330%。f1amb-1t載流子調(diào)控層的主要作用是通過其電子和空穴的雙極傳輸特性,有效的實(shí)現(xiàn)白光器件內(nèi)的載流子傳輸平衡;構(gòu)建flamb-1t/dcddc/flamb-1t載流子陷阱結(jié)構(gòu),采用直接載流子捕獲的方式實(shí)現(xiàn)dcddc紅光發(fā)射,從而調(diào)控載流子的復(fù)合中心,實(shí)現(xiàn)白光發(fā)射。當(dāng)flamb-1t為10nm時(shí),獲得commissioninternationaledel'eclairage(cie)坐標(biāo)為(0.33,0.36)的woleds。不同電壓驅(qū)動(dòng)下,最優(yōu)化的woleds載流子復(fù)合中心位置始終被限制在三個(gè)穩(wěn)定的區(qū)域,這說明flamb-1t載流子調(diào)控層可以有效的控制激子形成區(qū)域。3、研究有機(jī)電荷產(chǎn)生層的性能對(duì)串聯(lián)oleds性能的影響采用boronsubphthalocyaninechloride(subpc):fullerene(c60)和cobalt(ii)phthalocyanine(copc):c60兩種有機(jī)體異質(zhì)結(jié)電荷產(chǎn)生層,分別制備了高性能的串聯(lián)oleds,研究了電荷產(chǎn)生層載流子調(diào)控能力的優(yōu)化對(duì)串聯(lián)器件性能的影響。研究發(fā)現(xiàn),電荷產(chǎn)生層的優(yōu)化可以改善有機(jī)體異質(zhì)結(jié)界面,增加界面偶極子數(shù)量,提升電荷產(chǎn)生層的電荷產(chǎn)生能力;增加載流子傳輸通道,提升電荷產(chǎn)生層的載流子傳輸能力,促進(jìn)器件內(nèi)載流子的平衡傳輸,從而改善器件的性能。通過上述研究,優(yōu)化電荷產(chǎn)生層中給體subpc和copc的含量,獲得了最大電流效率分別為63.6cd/a和50.2cd/a串聯(lián)oleds。4、研究低溫?zé)嵬嘶饅no陰極修飾層對(duì)倒置型pscs性能的影響采用低溫?zé)嵬嘶鸸に囍苽溲趸�鋅(zincoxide,zno)陰極修飾層,研究zno的光電特性對(duì)ipscs載流子調(diào)控和器件性能的影響。研究發(fā)現(xiàn),真空動(dòng)態(tài)退火工藝可以改善zno薄膜的表面形貌,顯著降低的薄膜表面粗糙度這主要?dú)w因于熱流的分布情況、溶劑的揮發(fā)過程和zno前驅(qū)體的熱分解過程。采用真空動(dòng)態(tài)退火zno的倒置型器件的能量轉(zhuǎn)換效率(power-conversionefficiency,pce)為4.01%,相比原位退火zno的器件性能提升了15.8%,。真空動(dòng)態(tài)退火zno的作用是降低ito/活性層之間的接觸電阻,抑制漏電流的產(chǎn)生;同時(shí)有效控制器件內(nèi)載流子的復(fù)合過程,提升電子的傳輸和收集能力,從而改善器件的性能。綜上所述,本研究工作設(shè)計(jì)了具有載流子調(diào)控能力的若干種不同結(jié)構(gòu)的OLEDs,為實(shí)現(xiàn)高性能的器件奠定了理論基礎(chǔ)和提供了理論指導(dǎo)。同時(shí),具有載流子調(diào)控能力的Zn O功能層可以用來改善IPSC的器件性能。這表明載流子調(diào)控是實(shí)現(xiàn)高性能有機(jī)光電子器件的有效途徑。
[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.
【學(xué)位授予單位】：電子科技大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2016
【分類號(hào)】：TN383.1

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10 李春;可溶性有機(jī)小分子電致發(fā)光器件制備與性能研究[D];華南理工大學(xué);2011年

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