Modulation of half-band-gap turn-on electroluminescence in Rubrene/C<sub>60</sub> based OLEDs by electron injection layer mobility

Peng Teng; Wang Hui-Yao; Zhao Xi; Liu Jun-Hong; Wang Bo; Wang Jing-Jing; Zhou Yin-Qiong; Zhang Ke-Yi; Yang Jun; Xiong Zu-Hong

doi:10.7498/aps.73.20240864

Abstract

Half-band-gap turn-on characteristic is a unique photoelectric property of organic light-emitting diodes (OLEDs), and has advantage in the development of low driving voltage devices. But the physical mechanism that the electron injection layer (EIL) affects the half-band-gap turn-on characteristic has not been reported. In this work, the change from half-band-gap turn-on electroluminescence (EL) to sub-band-gap turn-on EL to normal turn-on EL is observed by regulating the electron mobility of EIL in Rubrene/C₆₀ based devices. Three sets of devices are fabricated by using BCP (~10^–3 cm²/(V·s), Dev. 1), Bphen (~10^–4 cm²/(V·s), Dev. 2) and TPBi (~10^–5 cm²/(V·s), Dev. 3) as EIL materials. By measuring the I-B-V curves of devices at room temperature, it is found that the turn-on voltages of devices obviously increase by an order of magnitude with electron mobility of EIL decreasing. Specifically, the turn-on voltage of Dev. 1, Dev. 2, and Dev. 3 exhibit the physical phenomena of half-band-gap turn-on (1.1 V), sub-band-gap turn-on (2.1 V) and normal turn-on (4.1 V) properties, respectively. The magneto-electroluminescence (MEL) results show that the half-band-gap turn-on characteristic of high EIL electron mobility (Dev. 1) is attributed to the triplet-triplet annihilation (TTA, T_1,Rb + T_1,Rb → S_1,Rb + S₀) process which can effectively reduce the turn-on voltage. However, the half-band-gap turn-on characteristic is not observed in the devices (Dev. 2 and Dev. 3) with low carrier mobility, which can be reasonably explained by a higher voltage that is applied to the EIL with low electron mobility in order to inject more electrons. The higher voltage offsets the reduced turn-on voltage of the TTA process, resulting in Dev. 2 and Dev. 3 with sub-band-gap turn-on and normal turn-on, respectively. In addition, although the TTA process is observed in all three devices, the TTA process is stronger and the EL is higher in Dev. 1 with high EIL electron mobility. This is because a large number of triplet Rubrene/C₆₀ exciplex states (EX₃) are formed at the Rubrene/C₆₀ interface, enhancing the Dexter energy transfer (DET, EX₃ → T_1,Rb) process from EX₃ to triplet exciton of Rubrene (T_1,Rb). That is, Dev. 1 exhibits stronger TTA process and higher EL due to the presence of a large number of T_1,Rb excitons formed by DET process than Dev. 2 and Dev. 3. Furthermore, by measuring the I-V curves of devices at low temperature, it is found that the reduced carrier mobility caused by lowering operational temperature increases the turn-on voltages of these three devices. The significantly different increases in the turn-on voltages of Dev. 1–3 at the same low temperature are due to the different influences of temperature on the electron mobility of EIL. The tradeoff between the decrease of carrier mobility and the extension of exciton lifetime makes the MEL curves present different temperature-dependent behaviors. This work further deepens the understanding of the influence of EIL electron mobility on the turn-on voltage and the related physical microscopic mechanism in Rubrene/C₆₀ devices.

Keywords:

Authors and contacts

Chongqing Key Laboratory of Micro & Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China

Corresponding author: Xiong Zu-Hong, zhxiong@swu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 12474074).

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References

[1]	D’Andrade B W, Esler J, Lin C, Adamovich V, Xia S, Weaver M S, Kwong R, Brown J J 2008 Proc SPIE 7051 70510Q Google Scholar
[2]	Reineke S, Lindner F, Schwartz G, Seidler N, Walzer K, Lussem B, Leo K 2009 Nature 459 234 Google Scholar
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Cited By

图 1 (a) 器件1—3的能级结构示意图; (b) 器件1—3的归一化EL谱; (c), (d) 室温下器件1—3的亮度-电压特性曲线和电流-电压特性曲线

Figure 1. (a) Energy level diagram of device 1–3; (b) normalized EL spectra of devices 1–3; (c), (d) the brightness-voltage and current-voltage curves of devices 1–3 at room temperature.

DownLoad: Full-Size Img PowerPoint

图 2 Rubrene/C₆₀型器件中激发态的微观演化过程, 其中插图分别展示了C₆₀和Rubrene的化学分子结构

Figure 2. Microscopic evolution processes of excited states occurring in the Rubrene/C₆₀ device. The inset shows the chemical molecular structure of C₆₀ and Rubrene.

DownLoad: Full-Size Img PowerPoint

图 3 (a)—(c) 器件1—3的微观机理示意图

Figure 3. (a)–(c) The schematic diagram of microscopic mechanisms occurring in devices 1–3.

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图 4 (a)—(c) 室温下器件1—3的MEL曲线

Figure 4. (a)–(c) The MEL curves of devices 1–3 at room temperature.

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图 5 (a)—(c) 器件1—3在不同温度下的电流-电压特性曲线; (d) 在300 K和100 K下器件1—3中电荷载流子的运输和复合过程的微观示意图

Figure 5. (a)–(c) Current-voltage curves of devices 1–3 at different operating temperatures; (d) schematic diagram of charge-carrier transport and recombination in devices 1–3 at 300 K and 100 K.

DownLoad: Full-Size Img PowerPoint

图 6 (a)—(c) 电流500 µA时器件1—3中温度依赖的MEL曲线

Figure 6. (a)–(c) Temperature-dependent MEL curves of devices 1–3 at bias current of 500 µA.

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表 1 器件1—3的具体结构

Table 1. Specific structure of devices 1–3.

Device name	Structure
Dev. 1	ITO/PEDOT:PSS/Rubrene (35 nm)/BCP (3 nm)/C₆₀ (50 nm)/BCP (10 nm)/LiF (1 nm)/Al (100 nm)
Dev. 2	ITO/PEDOT:PSS/Rubrene (35 nm)/BCP (3 nm)/C₆₀ (50 nm)/Bphen (10 nm)/LiF (1 nm)/Al (100 nm)
Dev. 3	ITO/PEDOT:PSS/Rubrene (35 nm)/BCP (3 nm)/C₆₀ (50 nm)/TPBi (10 nm)/LiF (1 nm)/Al (100 nm)

DownLoad: CSV

map

[1]	D’Andrade B W, Esler J, Lin C, Adamovich V, Xia S, Weaver M S, Kwong R, Brown J J 2008 Proc SPIE 7051 70510Q Google Scholar
[2]	Reineke S, Lindner F, Schwartz G, Seidler N, Walzer K, Lussem B, Leo K 2009 Nature 459 234 Google Scholar
[3]	Helander M G, Wang Z B, Qiu J, Greiner M T, Puzzo D P, Liu Z W, Lu Z H 2011 Science 332 944 Google Scholar
[4]	Komoda T, Yamae K, Kittichungchit V, Tsuji H, Ide N 2012 J. Photopolym. Sci. Technol. 25 321 Google Scholar
[5]	Pandey A K, Nunzi J M 2007 Adv. Mater. 19 3613 Google Scholar
[6]	Engmann S, Barito A J, Bittle E G, Giebink N C, Richter L J, Gundlach D J 2019 Nat. Commun. 10 227 Google Scholar
[7]	Chen Q S, Jia W Y, Chen L X, Yuan D, Zou Y, Xiong Z H 2016 Sci. Rep. 6 25331 Google Scholar
[8]	Tu L Y, Tang X T, Wang Y, Zhao X, Ma C H, Ye S N, Xiong Z H 2021 Phys. Rev. Appl. 16 064002 Google Scholar
[9]	Xiang C Y, Peng C, Chen Y, So F 2015 Small 11 5439 Google Scholar
[10]	He S J, Lu Z H 2016 J. Photonics Energy 6 036001 Google Scholar
[11]	Tang X T, Hu Y Q, Jia W Y, Pan R H, Deng J Q, He Z H, Xiong Z H 2018 ACS Appl. Mater. Interfaces 10 1948 Google Scholar
[12]	Yasuda T, Yamaguchi Y, Zou D C, Tsutsui T 2002 Jpn. J. Appl. Phys. 41 5626 Google Scholar
[13]	Wang Y P, Li B, Jiang C, Fang Y, Bai P, Wang Y 2021 J. Phys. Chem. C 125 16753 Google Scholar
[14]	Hung W Y, Ke T H, Lin Y T, Wu C C, Hung T H, Chao T C, Wong K T, Wu C I 2006 Appl. Phys. Lett. 88 064102 Google Scholar
[15]	Niu L B, Zhang Y, Chen L J, Zhang Q M, Guan Y X 2020 Org. Electron. 87 105971 Google Scholar
[16]	Jin P F, Zhou Z Y, Wang H, Hao J J, Chen R, Wang J Y, Zhang C 2022 J. Phys. Chem. Lett. 13 2516 Google Scholar
[17]	吴雨廷, 朱洪强, 魏福贤, 王辉耀, 陈敬, 宁亚茹, 吴凤娇, 陈晓莉, 熊祖洪 2022 71 227201 Google Scholar Wu Y T, Zhu H Q, Wei F X, Wang H Y, Chen J, Ning Y R, Wu F J, Chen X L, Xiong Z H 2022 Acta Phys. Sin. 71 227201 Google Scholar
[18]	Bai J W, Chen P, Lei Y L, Zhang Y, Zhang Q M 2014 Org. Electron. 15 169 Google Scholar
[19]	Piland G B, Burdett J J, Kurunthu D, Bardeen C J 2013 J. Phys. Chem. C 117 1224 Google Scholar
[20]	Crooker S A, Liu F, Kelley M R, Martinez N J D, Nie W, Mohite A, Nayyar I H, Tretiak S, Smith D L, Ruden P P 2014 Appl. Phys. Lett. 105 153304 Google Scholar
[21]	Geng R, Subedi R C, Luong H M, Pham M T, Huang W C, Li X G, Hong K L, Shao M, Xiao K, Hornak L A, Nguyen T D 2018 Phys. Rev. Lett. 120 086602 Google Scholar
[22]	Hosokawa C, Tokailin H, Higashi H, Kusumoto T 1992 Appl. Phys. Lett. 60 1220 Google Scholar
[23]	黄维, 密保秀, 高志强 2011 有机电子学 (北京: 科学出版社) 第300页 Huang W, Mi B X, Gao Z Q 2011 Organic Electronic (Beijing: Science Press) p300
[24]	Park B, In I, Gopalan P, Evans P G, King S, Lyman P F 2008 Appl. Phys. Lett. 92 133302 Google Scholar
[25]	Kobayashi S, Takenobu T, Mori S, Fujiwara A, Iwasa Y 2003 Sci. Technol. Adv. Mater. 4 371 Google Scholar
[26]	Peng Q, Chen P, Li F 2013 Appl. Phys. Lett. 102 023301 Google Scholar
[27]	Qiao X F, Yuan P S, Ma D G, Ahamad T, Alshehri S M 2017 Org. Electron. 46 1 Google Scholar
[28]	Lei Y L, Zhang Y, Liu R, Chen P, Song Q L 2009 Org. Electron. 10 889 Google Scholar
[29]	Liu Y, Wu X M, Zhao Z H, Gao J N, Zhan J, Rui H S, Lin X, Zhang N, Hua Y L, Yin S G 2017 Appl. Surf. Sci. 413 302 Google Scholar
[30]	Tang X T, Pan R H, Zhao X, Jia W Y, Wang Y, Ma C H 2020 Adv. Funct. Mater. 5 765 Google Scholar
[31]	王辉耀, 宁亚茹, 吴凤娇, 赵茜, 陈敬, 朱洪强, 魏福贤, 吴雨廷, 熊祖洪 2022 71 217201 Google Scholar Wang H Y, Ning Y R, Wu F J, Zhao X, Chen J, Zhu H Q, Wei F X, Wu Y T, Xiong Z H 2022 Acta Phys. Sin. 71 217201 Google Scholar
[32]	Wang Y, Ning Y R, Wu F G, Chen J, Chen X L, Xiong Z H 2022 Adv. Funct. Mater. 32 2202882 Google Scholar
[33]	宁亚茹, 赵茜, 汤仙童, 陈敬, 吴凤娇, 贾伟尧, 陈晓莉, 熊祖洪 2022 71 087201 Google Scholar Ning Y R, Zhao X, Tang X T, Chen J, Wu F J, Jia W R, Chen X L, Xiong Z H 2022 Acta Phys. Sin. 71 087201 Google Scholar
[34]	Peng Q M, Li A W, Fan Y X, Chen P, Li F 2014 J. Mater. Chem. C 2 6264 Google Scholar
[35]	陈秋松, 袁德, 贾伟尧, 陈历相, 邹越, 向杰, 陈颖冰, 张巧明, 熊祖洪 2015 64 177801 Google Scholar Chen Q S, Yuan D, Jia W Y, Chen L X, Zou Y, Xiang J, Chen Y B, Zhang Q M, Xiong Z H 2015 Acta Phys. Sin. 64 177801 Google Scholar

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Modulation of half-band-gap turn-on electroluminescence in Rubrene/C₆₀ based OLEDs by electron injection layer mobility

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Corresponding author: Xiong Zu-Hong, zhxiong@swu.edu.cn

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Modulation of half-band-gap turn-on electroluminescence in Rubrene/C60 based OLEDs by electron injection layer mobility

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Corresponding author: Xiong Zu-Hong, zhxiong@swu.edu.cn

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Modulation of half-band-gap turn-on electroluminescence in Rubrene/C₆₀ based OLEDs by electron injection layer mobility