溶液法制备的空穴传输层和注入层对有机电致发光器件性能的影响
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摘要
有机电致发光器件(OLED)在显示和照明等领域具有广泛的应用前景。虽然其在很多方面都具有优异的性能,但器件性能的进一步提高和器件机理的深入探索仍然是研究者努力的方向。空穴注入和传输能力是影响器件性能的重要因素,溶液法制备的空穴功能层可以简化器件的制备工艺并节省大量的能源。本论文系统研究了溶液法制备的V2O5、CuTCPc和PCDTBT空穴注入层或传输层对有机电致发光器件性能的提高及其原因,主要工作内容如下：
1、研究了利用V205饱和水溶液处理ITO对器件空穴注入能力的影响,并对器件性能提高原因的进行了探索。与紫外臭氧处理的器件相比,V205饱和水溶液处理后器件的电流密度和亮度相对较低,但其效率得到了提升。这主要是源于V205的存在对电荷传输平衡的影响,即V205在一定程度上增加空穴的注入,又防止空穴过度注入而造成的载流子不平衡。另外,交流阻抗测试表明,饱和V205水溶液浸泡处理ITO后器件的串联电阻明显变大,大于未做任何处理的器件以及紫外臭氧处理的器件。串联电阻的增大导致V2Os层分担了器件中的一部分电压,有利于空穴的隧穿注入。
2、研究了2,9,16,23-tetracarboxylic copper phthalocyanine (CuTCPc)空穴传输层对NPB/Alq3结构的有机电致发光器件性能的影响。CuTCPc空穴传输层的插入,不但提高器件了空穴的注入和传输能力,增加了器件的电流密度和亮度,还提高了器件的效率。一般认为,在NPB/Alq3结构的器件中,空穴载流子是多数载流子,空穴的增加将导致载流子不平衡从而降低器件效率；但是在此处采用CuTCPc器件中,增加空穴却仍然能提高器件的效率,这主要是由于器件驱动电压的降低。
同时,为了进一步探明电子或空穴注入对NPB/Alq3结构的有机电致发光器件性能的影响,我们利用一系列结构为NPB/Alq3:C545T/Alq3的器件,研究了器件中载流子复合区域的变化。结果发现,器件的发光没有出现光谱的变化,这表明注入的电子和空穴能较好的在掺杂层复合。并且发现不论增加电子注入,还是增加空穴输入,或者电子和空穴的注入都增加,都能提高器件的效率。
3、研究了PCDTBT作为空穴功能层材料在有机电致发光器件中的作用。PCDTBT为有机太阳能电池中常用的给体材料,利用PCDTBT:PVK作为空穴传输层,大幅度的提高PVK层的空穴传输能力,显著提高了器件的发光亮度,并且明显降低了器件的启亮电压。与未掺杂的器件相比,相同电流密度下器件亮度的提高达5倍之多。PCDTBT:PVK空穴传输层对器件的光谱有一定的影响,随着掺杂浓度的提高,器件中PCDTBT中发光峰的相对强度逐渐增强。并且,研究了PCDTBT掺杂PVK对有机电致发光器件中电场分布的影响,发现PCDTBT的掺杂不但增加了器件的电流,还减小了有机层中的电场强度。空穴的注入增多和器件中电场强度的降低,同样有利于器件效率的提高。
为了防止PCDTBT发光峰对器件性能的影响,又制备了ITO/PCDTBT/NPB/A1q3/LiF/Al结构的器件。当PCDTBT浓度较低时可以增加器件的电流密度和亮度,但是当其浓度过高时器件的电流密度和亮度下降。低浓度的PCDTBT修饰ITO导致器件电流增高是因为PCDTBT的能级结构可以形成阶梯势垒,有利于空穴的注入；高浓度PCDTBT修饰导致器件电流下降是由于PCDTBT迁移率相比于NPB要低,导致器件电阻变大不利于器件空穴的传输。
本文中共有图62幅,表7个,参考文献145篇。
Organic light emitting diodes (OLEDs) have been broadly used for displaying and lighting. Although OLEDs possess excellent properties, the improvement of device performance and the investigation in device physics are still hotpots and focuses in this research field. Hole injection and transporting are two of key factors determining the performances of OLEDs. Hole injection or transport layers prepared by a solution method can save a lot of energy, In this paper, various hole transport materials, including V2O5, CuTCPc and PCDTBT, are prepared from solutions. Meanwhile, the role of these materials and their effects on device performance are also investigated. The experiment results are obtained and listed as follows:
Firstly, the effect of indium tin oxide (ITO) modified by vanadium penoxide (V2O5) saturation solution was studied. It is found that the V2O5solution-treated devices have a much higher current density compared to the device with bare ITO and a higher current efficiency compared with UV-ozone-treated device. Series resistances were derived by fitting the current-voltage curves and monitoring the AC impedance. The influence of series resistances were also taken into account in this section.
Secondly, the effects of a hole-transport layer2,9,16,23-tetracarboxylic copper phthalocyanine (CuTCPc) using a spin-coating way was investigated The insertion of the CuTCPc between ITO and N,N'-biphenyl-N,N'-bis (1-naphthyl)-(1,1'-biphenyl)-4,4'-diamine (NPB) significantly reduces the operating voltage and thereby increases the current efficiency. The hole is considered to be the main carrier in NPB/Alq3structure devices, but the increase of hole-transporting can still improve the efficiency of the devices. In this case, the use of the hole transport layer CuTCPc can greatly abate the average field intensity in the devices, thus diminish the negative impact of carrier imbalance.
The effect of the device structure of NPB/A1Q3:C545T/AlQ3was also studied. Considering that the hole is the major carrier in this structure, the enhanced hole injection is attributed to the imbalance of different carriers and lower efficiency. However, in our study, it indicates that the current efficiency increases with the increasing of the hole concentration. We speculate that the increased current efficiency comes from a lower average electric field due to the hole transport layer CuTCPc in the devices.
Finally, we doped PCDTBT (Poly [[9-(l-octylnonyl)-9H-carbazole-2,7-diyl]-2, 5-thiophenediyl-2,1,3-benzothiadiazole-4,7-diyl-2,5-thiophenediyl]), a kind of Poly carbazole compounds, into the commonly used hole transport layer (HTL) PVK. The doped PCDTBT in PVK can significantlyenhance the luminance and reduce the turn-on voltage of the devices. The proportion of the PCDTBT peak becomes gradually larger along with the increase of the doping concentration of PCDTBT, and the device with the largest doped concentration achieved five times higher brightness compared to the as-spun device.
In order to prevent the luminescence of PCDTBT, we studied the devices with the structure of ITO/PCDTBT/NPB/Alq3/LiF/Al. We found that the turn-on voltage was reduced with increasing PCDTBT concentration. At a high voltage, the current density first increased and then decreased with the increase of PCDTBT concentration implying that the inserted PCDTBT layer improved the hole injection ability but reduced its hole transport ability.
1、研究了利用V205饱和水溶液处理ITO对器件空穴注入能力的影响,并对器件性能提高原因的进行了探索。与紫外臭氧处理的器件相比,V205饱和水溶液处理后器件的电流密度和亮度相对较低,但其效率得到了提升。这主要是源于V205的存在对电荷传输平衡的影响,即V205在一定程度上增加空穴的注入,又防止空穴过度注入而造成的载流子不平衡。另外,交流阻抗测试表明,饱和V205水溶液浸泡处理ITO后器件的串联电阻明显变大,大于未做任何处理的器件以及紫外臭氧处理的器件。串联电阻的增大导致V2Os层分担了器件中的一部分电压,有利于空穴的隧穿注入。
2、研究了2,9,16,23-tetracarboxylic copper phthalocyanine (CuTCPc)空穴传输层对NPB/Alq3结构的有机电致发光器件性能的影响。CuTCPc空穴传输层的插入,不但提高器件了空穴的注入和传输能力,增加了器件的电流密度和亮度,还提高了器件的效率。一般认为,在NPB/Alq3结构的器件中,空穴载流子是多数载流子,空穴的增加将导致载流子不平衡从而降低器件效率；但是在此处采用CuTCPc器件中,增加空穴却仍然能提高器件的效率,这主要是由于器件驱动电压的降低。
同时,为了进一步探明电子或空穴注入对NPB/Alq3结构的有机电致发光器件性能的影响,我们利用一系列结构为NPB/Alq3:C545T/Alq3的器件,研究了器件中载流子复合区域的变化。结果发现,器件的发光没有出现光谱的变化,这表明注入的电子和空穴能较好的在掺杂层复合。并且发现不论增加电子注入,还是增加空穴输入,或者电子和空穴的注入都增加,都能提高器件的效率。
3、研究了PCDTBT作为空穴功能层材料在有机电致发光器件中的作用。PCDTBT为有机太阳能电池中常用的给体材料,利用PCDTBT:PVK作为空穴传输层,大幅度的提高PVK层的空穴传输能力,显著提高了器件的发光亮度,并且明显降低了器件的启亮电压。与未掺杂的器件相比,相同电流密度下器件亮度的提高达5倍之多。PCDTBT:PVK空穴传输层对器件的光谱有一定的影响,随着掺杂浓度的提高,器件中PCDTBT中发光峰的相对强度逐渐增强。并且,研究了PCDTBT掺杂PVK对有机电致发光器件中电场分布的影响,发现PCDTBT的掺杂不但增加了器件的电流,还减小了有机层中的电场强度。空穴的注入增多和器件中电场强度的降低,同样有利于器件效率的提高。
为了防止PCDTBT发光峰对器件性能的影响,又制备了ITO/PCDTBT/NPB/A1q3/LiF/Al结构的器件。当PCDTBT浓度较低时可以增加器件的电流密度和亮度,但是当其浓度过高时器件的电流密度和亮度下降。低浓度的PCDTBT修饰ITO导致器件电流增高是因为PCDTBT的能级结构可以形成阶梯势垒,有利于空穴的注入；高浓度PCDTBT修饰导致器件电流下降是由于PCDTBT迁移率相比于NPB要低,导致器件电阻变大不利于器件空穴的传输。
本文中共有图62幅,表7个,参考文献145篇。
Organic light emitting diodes (OLEDs) have been broadly used for displaying and lighting. Although OLEDs possess excellent properties, the improvement of device performance and the investigation in device physics are still hotpots and focuses in this research field. Hole injection and transporting are two of key factors determining the performances of OLEDs. Hole injection or transport layers prepared by a solution method can save a lot of energy, In this paper, various hole transport materials, including V2O5, CuTCPc and PCDTBT, are prepared from solutions. Meanwhile, the role of these materials and their effects on device performance are also investigated. The experiment results are obtained and listed as follows:
Firstly, the effect of indium tin oxide (ITO) modified by vanadium penoxide (V2O5) saturation solution was studied. It is found that the V2O5solution-treated devices have a much higher current density compared to the device with bare ITO and a higher current efficiency compared with UV-ozone-treated device. Series resistances were derived by fitting the current-voltage curves and monitoring the AC impedance. The influence of series resistances were also taken into account in this section.
Secondly, the effects of a hole-transport layer2,9,16,23-tetracarboxylic copper phthalocyanine (CuTCPc) using a spin-coating way was investigated The insertion of the CuTCPc between ITO and N,N'-biphenyl-N,N'-bis (1-naphthyl)-(1,1'-biphenyl)-4,4'-diamine (NPB) significantly reduces the operating voltage and thereby increases the current efficiency. The hole is considered to be the main carrier in NPB/Alq3structure devices, but the increase of hole-transporting can still improve the efficiency of the devices. In this case, the use of the hole transport layer CuTCPc can greatly abate the average field intensity in the devices, thus diminish the negative impact of carrier imbalance.
The effect of the device structure of NPB/A1Q3:C545T/AlQ3was also studied. Considering that the hole is the major carrier in this structure, the enhanced hole injection is attributed to the imbalance of different carriers and lower efficiency. However, in our study, it indicates that the current efficiency increases with the increasing of the hole concentration. We speculate that the increased current efficiency comes from a lower average electric field due to the hole transport layer CuTCPc in the devices.
Finally, we doped PCDTBT (Poly [[9-(l-octylnonyl)-9H-carbazole-2,7-diyl]-2, 5-thiophenediyl-2,1,3-benzothiadiazole-4,7-diyl-2,5-thiophenediyl]), a kind of Poly carbazole compounds, into the commonly used hole transport layer (HTL) PVK. The doped PCDTBT in PVK can significantlyenhance the luminance and reduce the turn-on voltage of the devices. The proportion of the PCDTBT peak becomes gradually larger along with the increase of the doping concentration of PCDTBT, and the device with the largest doped concentration achieved five times higher brightness compared to the as-spun device.
In order to prevent the luminescence of PCDTBT, we studied the devices with the structure of ITO/PCDTBT/NPB/Alq3/LiF/Al. We found that the turn-on voltage was reduced with increasing PCDTBT concentration. At a high voltage, the current density first increased and then decreased with the increase of PCDTBT concentration implying that the inserted PCDTBT layer improved the hole injection ability but reduced its hole transport ability.
引文
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