激基复合物与电致激基复合物共存体系中Dexter能量传递导致的负磁效率

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

doi:10.7498/aps.71.20221288

摘要

因具有反向系间窜越过程(reverse intersystem crossing, RISC)在低成本就可实现高效率发光, 激基复合物(exciplex)型有机发光二极管(organic light-emitting diodes, OLEDs)是目前的一个研究热点. 其微观过程通常表现为极化子对的系间窜越(ISC)过程占主导, 引起的磁电致发光(magneto-electroluminescence, MEL)效应和磁电导(magneto-conductance, MC)效应都是正值, 且MEL幅值大于MC幅值; 由于在一般电流(I)范围内存在线形关系EL $ \propto \eta \cdot I $, 对应的磁效率(magneto-efficiency, Mη)也是正值. 本工作却在激基复合物与电致激基复合物(electroplex)共存的器件中发现: 虽然在小电流下MEL值也大于MC值, 但是电流增大后MEL值逐渐小于MC值, 即Mη值由正变成负. 通过对比该型器件与纯激基复合物型器件中不同的物理微观过程发现: 激基复合物与电致激基复合物共存器件中存在从激基复合物到电致激基复合物的Dexter能量转移(Dexter energy transfer, DET)过程, 此过程会增强电致激基复合物的RISC过程, 且DET过程会随电流的增大而增强, 导致器件在大电流下表现为RISC过程主导的负Mη. 本工作有助于认识激基复合物型OLEDs中激发态间的相互作用规律, 也为制作高效率发光器件提供了理论参考.

关键词:

Abstract

Exciplex-type organic light-emitting diodes (OLEDs) are research focus at present, because of their high-efficiency luminescence at low cost due to the reverse intersystem crossing (RISC, EX₁ ← EX₃). Their microscopic processes usually exhibit intersystem crossing (ISC, PP₁ → PP₃) process dominated by polar pairs, leading the magneto-electroluminescence [MEL, MEL = (ΔEL)/EL × 100%] effect values and the magneto-conductance [MC, MC = (ΔI)/I × 100%] effect values to be both positive, the amplitude of MEL to be greater than that of MC at the same current, and the corresponding magnetic efficiency [Mη, Mη = (Δη)/η × 100%] values to be also positive due to the linear relationship EL $ \propto \eta\cdot I $ within general current (I) range. Surprisingly, although the MEL value of the device coexisting with exciplex and electroplex is also greater than the MC value at low current, MEL value is less than MC value at high current. In other words, Mη value of this device undergoes a conversion from positive to negative with current increasing. In this work, to find out the reason why Mη value of exciplex-type OLED formed by TAPC and TPBi shows a negative value under high current and also to study the micro-dynamic evolution mechanism of spin-pair states in this device, three OLEDs are fabricated and their luminescence spectra and organic magnetic field effect curves are measured. The results indicate that the electroplex is produced in the exciplex-type OLED formed by TAPC and TPBi. Since the triplet exciton energy of monomers TAPC and TPBi is higher than those of triplet charge-transfer states of exciplex (CT${}_3^{\rm{ex}} $), and the CT${}_3^{\rm{ex}} $ energy is greater than the energy of triplet charge-transfer states of electroplex (CT${}_3^{\rm{el}} $), the CT${}_3^{\rm{ex}} $ energy can only be transferred to CT${}_3^{\rm{el}} $ through Dexter energy transfer (DET) process without other loss channels. The electroluminescence (EL) spectrum of this device shows that the luminescence intensity of exciplex is greater than that of electroplex, which indicates that the quantity of exciplex is more than that of electroplex. Besides, EL spectra at different currents prove that the formation rate of exciplex is faster than that of electroplex with current increasing. Owing to less quantity of exciplex at low current, the DET process from CT${}_3^{\rm{ex}} $ to CT${}_3^{\rm{el}} $ is too weak to facilitate the RISC process of charge-transfer states of electroplex (CT^el). Therefore, the low field amplitude of Mη curve is positive at low current. The number of spin-pair states of exciplex increases with current increasing, which enhances the DET process. These processes of direct charge carriers trapped and energy transferred critically increase the number of CT${}_3^{\rm{el}} $ at high current, which greatly strengthens the RISC process of CT^el. Therefore, the low field amplitude of Mη curve changes from positive to negative with current increasing. Furthermore, the Mη curves of this device are measured when only exciplex exists and only electroplex exists in the employing filter, respectively. As expected, the results confirm the accuracy of the mechanism of the negative value of the total Mη for this device. Obviously, this work contributes to the comprehension of the internal micro-physical mechanism in OLEDs and the law of interactions between excited states.

Keywords:

作者及机构信息

1.
西南大学物理科学与技术学院, 微纳结构光电子学重庆市重点实验室, 重庆　400715

2.
重庆师范大学物理与电子工程学院, 光电功能材料重庆市重点实验室, 重庆　401331

通信作者: 朱洪强, 20132013@cqnu.edu.cn ; 熊祖洪, zhxiong@swu.edu.cn

基金项目: 重庆市教委科技项目(批准号: KJQN202200569)、国家自然科学基金(批准号: 12104076, 11874305)、重庆自然科学基金(批准号: cstc2019jcyj-msxmX0560)和重庆师范大学校级基金(批准号: 21XLB050)资助的课题.

Authors and contacts

1.
School of Physical Science and Technology, Chongqing Key Laboratory of Micro & nano Structure Optoelectronics, Southwest University, Chongqing 400715, China

2.
School of Physics and Electronic Engineering, Chongqing Key Laboratory of Optoelectronic Functional Materials, Chongqing Normal University, Chongqing 401331, China

Corresponding author: Zhu Hong-Qiang, 20132013@cqnu.edu.cn ; Xiong Zu-Hong, zhxiong@swu.edu.cn

Funds: Project supported by the Science and Technology Research Program of Chongqing Municipal Education Commission (Grant No. KJQN202200569), the National Natural Science Foundation of China (Grant Nos. 12104076, 11874305), the Chongqing Natural Science Foundation project (Grant No. cstc2019jcyj-msxmX0560) and the University-level Foundation of Chongqing Normal University (Grant No. 21XLB050).

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 能级结构和光谱 (a), (d) 器件1; (b), (e) 器件2; (c), (f) 器件3

Fig. 1. Energy level structures and luminance intensity: (a), (d) Device 1; (b), (e) device 2; (c), (f) device 3.

下载: 全尺寸图片幻灯片

图 2 (a)—(c) 室温下不同电流时器件1的MC, MEL和Mη曲线; (d) 它们的低场幅值随电流的变化规律; (e) 器件1的微观机理图

Fig. 2. (a)–(c) The current-dependent MC, MEL and Mη curves of device 1 at room temperature; (d) their low magnetic field values as a function of current; (e) microscopic mechanisms in device 1.

下载: 全尺寸图片幻灯片

图 3 (a)—(c) 器件2和(d)—(f) 器件3室温下不同电流时的MC, MEL和Mη曲线

Fig. 3. The current-dependent MC, MEL and Mη curves of device 2 (a)–(c) and device 3 (d)–(f) at room temperature.

下载: 全尺寸图片幻灯片

图 4 (a)器件2和(b)器件3的微观机理图

Fig. 4. Microscopic mechanisms in device 2 (a) and device 3 (b).

下载: 全尺寸图片幻灯片

图 5 (a)器件2和(b)器件3在室温下不同电流时的归一化EL谱; 器件3中(c)激基复合物和(d)电致激基复合物的Mη曲线

Fig. 5. The normalized current-dependent EL spectra of device 2 (a) and device 3 (b) at room temperature; Mη curves of exciplex (c) and electroplex (d) for device 3.

下载: 全尺寸图片幻灯片

[1]	Godlewski J, Obarowska M 2007 Eur. Phys. J. -Spec. Top. 144 51 Google Scholar
[2]	Pan Y Y, Li W J, Zhang S T, Yao L, Gu C, Xu H, Yang B, Ma Y G 2014 Adv. Opt. Mater. 2 510 Google Scholar
[3]	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
[4]	Uoyama H, Goushi K, Shizu K, Nomura H, Adachi C 2012 Nature 492 234 Google Scholar
[5]	Liu F L, Kelley M R, Crooker S A, Nie W Y, Mohite A D, Ruden P P, Smith D L 2014 Phys. Rev. B 90 235314 Google Scholar
[6]	Kalinowski J, Cocchi M, Virgili D, Marco P D, Fattori V 2003 Chem. Phys. Lett. 380 710 Google Scholar
[7]	Zhang T T, Holford D F, Gu H, Kreouzis T, Zhang S J, Gillin W P 2016 Appl. Phys. Lett. 108 023303 Google Scholar
[8]	Zhang L Cheah K W 2018 Sci. Rep. 8 8832 Google Scholar
[9]	Bera K, Douglas C J, Frontiera R R 2017 J. Phys. Chem. Lett. 8 5929 Google Scholar
[10]	赵茜, 汤仙童, 潘睿亨, 许静, 屈芬兰, 熊祖洪 2019 科学通报 64 2514 Google Scholar Zhao X, Tang X T, Pan R H, Xu J, Qu F L, Xiong Z H 2019 Chin. Sci. Bull. 64 2514 Google Scholar
[11]	Doubleday C, Turro N J, Wang J F 1989 Acc. Chem. Res. 22 199 Google Scholar
[12]	张勇, 刘亚莉, 焦威, 陈林, 熊祖洪 2012 物理学报 61 117106 Google Scholar Zhang Y, Liu Y L, Jiao W, Chen L, Xiong Z H 2012 Acta Phys. Sin. 61 117106 Google Scholar
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[17]	Wang Y F, Sahin-Tiras K, Harmon H J, Wohlgenannt M, Flatté M E 2016 Phys. Rev. X 6 011011 Google Scholar
[18]	Zhao X, Tang X T, Zhu H Q, Ma C H, Wang Y, Ye S N, Tu L Y, Xiong Z H 2021 ACS Appl. Electron. Mater. 3 3034 Google Scholar
[19]	Zhang T Y, Chu B, Li W L, Su Z S, Peng Q M, Zhao B, Luo Y S, Jin F M, Yan X W, Gao Y, Wu H R, Zhang F, Fan D, Wang J B 2014 ACS Appl. Mater. Interfaces 6 11907 Google Scholar
[20]	Gruenbaum W T, Sorriero L J, Borsenberger P M, Zumbulyadis N 1996 Jpn. J. Appl. Phys. 35 2714 Google Scholar
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[23]	Deng J Q, Jia W Y, Chen Y B, Liu D Y, Hu Y Q, Xiong Z H 2017 Sci. Rep. 7 44396 Google Scholar
[24]	Sheng Y, Nguyen T D, Veeraraghavan G, Mermer Ö, Wohlgenannt M, Qiu S, Scherf U 2006 Phys. Rev. B 74 045213 Google Scholar
[25]	Yuan P S, Qiao X F, Yan D H, Ma D G 2018 J. Mater. Chem. C 6 5721 Google Scholar
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[28]	宁亚茹, 赵茜, 汤仙童, 陈敬, 吴凤娇, 贾伟尧, 陈晓莉, 熊祖洪 2022 物理学报 71 087201 Google Scholar Ning Y R, Zhao X, Tang X T, Chen J, Wu F J, Jia W Y, Chen X L, Xiong Z H 2022 Acta Phys. Sin. 71 087201 Google Scholar
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[33]	Liu X K, Chen Z, Zheng C J, Liu C L, Lee C S, Li F, Ou X M, Zhang X H 2015 Adv. Mater. 27 2378 Google Scholar
[34]	Hu B, Wu Y 2007 Nat. Mater. 6 985 Google Scholar
[35]	Bagnich S A, Niedermeier U, Melzer C, Sarfert W, von Seggern H 2009 J. Appl. Phys. 106 113702 Google Scholar
[36]	Fan Y X, Sun A H, Tian Y H, Zhou P C, Niu Y X, Shi Wei, Wei B 2022 J. Phys. D: Appl. Phys. 55 315103 Google Scholar
[37]	Xu Z, Gong Y B, Dai Y F, Sun Q, Qiao X F, Yang D Z, Zhan X J, Li Z, Tang B Z, Ma D G 2019 Adv. Opt. Mater. 7 1801539 Google Scholar
[38]	Wu Z B, Wang Q, Yu L, Chen J S, Qiao X F, Ahamad T, Alshehri S M, Yang C L, Ma D G 2016 ACS Appl. Mater. Interfaces 8 28780 Google Scholar
[39]	Mondal A, Paterson L, Cho J, et al. 2021 Chem. Phys. Rev. 2 031304 Google Scholar

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