Carrier ladder effect regulated dissociation and scattering of triplet excitons in OLED

Bao Xi; Guan Yun-Xia; Li Wan-Jiao; Song Jia-Yi; Chen Li-Jia; Xu Shuang; Peng Ke-Ao; Niu Lian-Bin

doi:10.7498/aps.72.20230851

Abstract

Triplet exciton-charge interaction (TQI) has two forms: dissociation and scattering, However, it is still unclear how the hole injection layer affects the dissociation and scattering of triplet excition and the transition between positive and negative values of magneto-conductance (MC). In this paper, HAT-CN, which can produce carrier ladder effect, is used as hole injection layer (HIL), and magnetic effect is used as a tool to study it. The results show that there are three characteristic magnetic fields in the device: hyperfine, dissociation and scattering, which are verified by fitting the MC with Lorentzian and non-Lorentzian functions. The hyperfine characteristic magnetic field results from the magnetic field suppressing superfine field-induced charge-spin mixing. With the enhancement of magnetic field, hole injection layer/hole transport layer interface produces carrier ladder effect, which improves the hole injection efficiency. The triplet excitions are separated by the hole, then the secondary carriers are produced, which makes the device’s luminous brightness and efficiency reach to 43210 cd/m² and 9.8 cd/A, respectively. The carrier ladder effect will also lead to a large accumulation of injected charges, resulting in the scattering of charge carriers by triplet excition, thereby reducing their mobility, which is not conducive to the formation of excited states nor device luminescence. The MC is modulated by K_S/K_T (recombination rate ratio), and when the electric field is small $ {K}_{{\rm{S}}}\gg {K}_{{\rm{T}}} $, the recombination ratio is relatively large, resulting in positive MC. With the increase of electric field $ {K}_{{\rm{S}}}\approx {K}_{{\rm{T}}}=K$, K_S/K_T approaches 1 at this time, resulting in an MC, which is negative in a low temperature environment. This work provides a novel approach for regulating and effectively utilizing triplet excitons.

Keywords:

Authors and contacts

Chongqing Key Laboratory of Optical Engineering, Chongqing Key Laboratory of Optoelectronic Functional Materials, College of Physics and Electronic Engineering, Chongqing Normal University, Chongqing 400715, China

Corresponding author: Guan Yun-Xia, utk_lili@126.com ; Niu Lian-Bin, niulb03@126.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 61874016), the Natural Science Foundation Project of Chongqing, China (Grant Nos. CSTC2020jcyj-msxmX0282, CSTC2021jcyj-msxmX0576), and the Scientific and Technological Research Program of Chongqing Municipal Education Commission, China (Grant No. KJQN202200518).

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References

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Cited By

图 1 (a) MoO₃, PEDOT:PSS, HAT-CN, NPB分子结构; (b) 器件1—4的归一化电致发光谱图, 插图为发光峰局部放大图; (c) 器件4的器件结构图能级及电荷产生原理图; (d)器件1—4的亮度-电压曲线; (e)器件1—4的电流效率-电流密度曲线; (f) 器件4的界面ITO/HAT-CN/NPB能级排列图^[4]

Figure 1. (a) Molecular structure of MoO₃, PEDOT:PSS, HAT-CN, NPB; (b) normalized EL spectra of devices 1–4, illustrated as local magnification of luminous peaks; (c) device structure diagram and charge generation schematic diagram of device 4; (d) luminance-voltage curves of devices 1–4; (e) current efficiency-current density curves of devices 1–4; (f) ITO/HAT-CN/NPB energy level arrangement diagram at the interface of device 4 ^[4].

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图 2 常温时器件4 的磁效应　(a) 3—5 V时的MC(蓝色系曲线), MEL(绿色系曲线); (b) 3 V时0 mT < |B| < 50 mT范围内MC曲线; (c) 电流密度-电压线性拟合曲线; (d) 内部微观机制反应原理; 其中TF(LT)表示低温条件时发生三线态-三线态激子湮灭过程; q为电荷; ∆E为能极差; S₀为基态; ¹PP和³PP分别为单线态极化子和三线态极化子; k_coll为三线态激子和电荷相遇的速率常数; k_scat, k_diss, k_quen分别为散射通道、解离通道和淬灭通道的速率常数.

Figure 2. Magneto-effect of device 4 at room temperature: (a) MC (blue curve) and MEL (green curve) at 3–5 V; (b) the MC curve within the scope of 0 mT < |B| < 50 mT at 3 V; (c) linear fitting curve of current density-voltage; (d) reaction principle of internal microscopic mechanism. TF(LT) represents the triplet-triplet exciton annihilation process at low temperature. q is the charge. ∆E is the energy range. S₀ is the ground state. ¹PP and ³PP are singlet polaron and triplet polaron respectively. k_coll is the rate constant at which triplet exciton and charge meet. k_scat, k_diss and k_quen are the rate constants of scattering channel, dissociation channel and quenching channel, respectively.

DownLoad: Full-Size Img PowerPoint

图 3 (a)—(d) 器件1—4在偏置电压为6 V时的MC实验曲线及拟合曲线; (a)—(c) 插图分别为器件1—3的结构及能级图

Figure 3. MC experimental curves and fitting curves of (a)–(d) devices 1–4 when the bias voltage is 6 V; (a)–(c) illustrations are the structure and energy level diagrams of devices 1–3 respectively.

DownLoad: Full-Size Img PowerPoint

图 4 在300, 195, 95 K下, (a)—(c) 注入电流强度分为400, 600, 800 μA时器件4的MC曲线; (d) 电流-电压曲线, 插图为亮度-电压曲线

Figure 4. (a)–(c) MC curves of device 4 at 300, 195, 95 K with current of 400, 600, 800 μA; (d) current-voltage curves, where the inset shows the lightness-voltage curve.

DownLoad: Full-Size Img PowerPoint

图 5 (a)—(d) HAT-CN厚度为5—20 nm时, 电压为3, 4, 5, 6 V下的MC图; (e) 磁场为200 mT时, 不同偏压下的MC曲线; (f) 4类器件的效率比较图

Figure 5. (a)–(d) MC diagram with the voltage of 3, 4, 5, 6 V when the thickness of HAT-CN is 5—20 nm; (e) MC curves with a magnetic field of 200 mT and different bias voltages; (f) efficiency comparison diagram of four types of devices.

DownLoad: Full-Size Img PowerPoint

[1]	Yuan J K, Dai Y F, Sun Q, Qiao X F, Yang D Z, Chen J S, Ma D G 2019 Semicond. Sci. Technol. 34 105010 Google Scholar
[2]	Chang Q, Lü Z Y, Yin Y H, Xiao J, Wang J L 2022 Displays 75 102306 Google Scholar
[3]	Oh E, Park S, Jeong J, Kang J S, Lee H, Yi Y 2017 Chem. Phys. 668 64
[4]	Liu Z Y, Wei P C, Bin Z Y, Wang X W, Zhang D D, Duan L 2021 Sci. China Mater. 64 3124 Google Scholar
[5]	Park H G, Park S G 2019 Coatings 9 648 Google Scholar
[6]	Chen Y B, Jia W Y, Xiang J, Yuan D, Chen Q S, Chen L X, Xiong Z H 2016 Org. Electron. 39 207
[7]	Hu B, Yue W 2003 Nat. Mater. 6 985 Google Scholar
[8]	Desai P , Shakya P , Kreouzis T, Gillin W P, Morley N A, Gibbs M R J 2007 Phys. Rev. B 75 094423 Google Scholar
[9]	Shao M, Yan L , Li M X, Llia I, Hu B 2013 J. Mater. Chem. C 1 1330 Google Scholar
[10]	Park C H, Kang S W, Jung S G, Lee J D, Park Y W, Ju B K 2021 Sci. Rep. 11 3430 Google Scholar
[11]	Wu F J, Zhao X, Zhu H Q, Tang X T, Ning Y R, Chen J, Chen X L, Xiong Z H 2022 ACS Photonics 9 2713 Google Scholar
[12]	Mischok A, Hillebrandt S, Kwon S, Cather M C 2023 Nat. Photonics 17 393 Google Scholar
[13]	Niu L B, Zhong Y, Chen L J, Zhang Q M, Guan Y X 2020 Org. Electron. 87 105971 Google Scholar
[14]	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 物理学报 71 217201 Google Scholar Wang H Y, Ning Y R, Wu F J, Zhao Q, Chen J, Zhu H Q, Wei F X, Wu Y T, Xiong Z H 2022 Acta Phys. Sin. 71 217201 Google Scholar
[15]	Huh J S, Sung M J, Kwon S K, Kim Y H, Kim J J 2021 Adv. Funct. Mater. 31 2100967 Google Scholar
[16]	Deng Z B, Lee S T, Webb D P, Chan Y C, Gambling W A 1999 Synth. Met. 107 107 Google Scholar
[17]	Kepler R G, Beeson P M, Jacobs S J, Anderson R A, Sinclair M B, Valencia V S, Cahill P A 1995 Appl. Phys. Lett. 66 3618 Google Scholar
[18]	Chen B J, Lai W Y, Gao Z Q, Lee C S, Lee S T, Gambling W A 1999 Appl. Phys. Lett. 75 4010 Google Scholar
[19]	Lee H, Cho S W, Yi Y 2016 Curr. Appl. Phys. 16 1533 Google Scholar
[20]	Ding L, Sun Y Q, Chen H, Zu F S, Wang Z K, Liao L S 2014 J. Mater. Chem. C 2 10403 Google Scholar
[21]	Weng Z C, Gillin W P, Kreouzis T 2019 Sci. Rep. 9 3439 Google Scholar
[22]	Van Eersel, H, Bobbert P S, Janssen R A J, Coehoorn R 2016 J. Appl. Phys. 119 163102 Google Scholar
[23]	Hu B, Yan L, Shao M 2009 Adv. Mater. 21 1500
[24]	Bi H, Huo C Y, Song X X, Li Z Q, Tang H N, Griesse-Nascimento S, Huang K C, Cheng J X, Nienhaus L, Bawendi M G, Lin H Y G, Wang Y, Saikin S K 2020 J. Phys. Chem. Lett. 11 9364 Google Scholar
[25]	Hayashi H, Sakaguchi Y, Wakasa M 2001 Bull. Chem. Soc. Jpn. 74 773 Google Scholar
[26]	Kersten S P, Schellekens A J, Koopmans B, Bobbert P A 2011 Phys. Rev. Lett. 106 197402 Google Scholar
[27]	Jia W Y, Zhang Q M, Chen L J, Ling Y Z, Liu H, Lu C L, Chen P, Xiong Z H 2015 Org. Electron. 22 210 Google Scholar
[28]	Mark P, Helfrich W 1962 J. Appl. Phys. 33 205 Google Scholar
[29]	Wohlgenannt M, Vardeny Z V 2003 J. Phys-condens. Mat. 15 R83 Google Scholar
[30]	Gärditz C, Mückl A G, Cölle M 2005 J. Appl. Phys. 98 104507 Google Scholar
[31]	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. Inter. 10 1948 Google Scholar
[32]	Zhang Q M, Chen L J, Jia W Y, Lei Y L, Xiong Z H 2016 Org. Electron. 39 318 Google Scholar
[33]	Obolda A, Peng Q M, He C Y, Zhang T, Ren J J, Ma H W, Shuai Z G, Li F 2016 Adv. Mater. 28 4740 Google Scholar
[34]	Tsai K W, Lee T H, Wu J H, Jhou J Y, Huang W S, Hsieh S N, Wen T C, Guo T F, Huang, J C A 2013 Org. Electron. 14 1376 Google Scholar
[35]	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 Q, 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
[36]	Yuan P S, Qiao X F, Yan D H, Ma D G 2019 J. Mater. Chem. C 7 1035 Google Scholar
[37]	Ern V, Merrifield R E 1968 Phys. Rev. Lett. 21 609 Google Scholar
[38]	Zhang Z, Yates Jr J T 2012 Chem. Rev. 112 5520 Google Scholar
[39]	Jensen K L 2003 J. Vac. Sci. Technol. B. 21 1528

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