Exciton regulation mechanism of Alq<sub>3</sub>/HAT-CN tandem electroluminescent devices

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

doi:10.7498/aps.72.20230973

Abstract

Tandem organic electroluminescent devices (OLEDs) have attracted widespread attention due to their long lifetime and high current efficiency. In this study, a double-emitting unit tandem OLED is fabricated by using Alq₃/HAT-CN as an interconnect layer. Its photovoltaic properties and exciton regulation mechanism are investigated. The results show that the luminance (11189.86 cd/m²) and efficiency (13.85 cd/A) of the tandem OLED reaches 2.7 times that of the single electroluminescent (EL) unit OLED (luminance and efficiency of 4007.14 cd/m² and 5.00 cd/A, respectively) at a current density of 80 mA/cm². This proves that the Alq₃/HAT-CN is an efficient interconnect layer. At room temperature, the polaron pair undergoes intersystem crossing (ISC) due to hyperfine interaction (HFI) when a magnetic field is applied to the device. This increases the concentration of the triplet excitons (T₁), thus promoting the charge scattering. The result is a rapid increase in the low magnetic field and a slow increase in the high magnetic field of the MEL. When the injection current strength is constant, there is less uncompounded charge in the Alq₃/HAT-CN device than in other connected layer devices. Triplet-charge annihilation (TQA) is weak, resulting in a relative increase in the value of T₁, which is not involved in the TQA. This suppresses the ISC and leads to a minimal increase in the MEL. As the current strength increases, the T₁ value increases, causing TQA to increase and ISC to decrease. Since the TQA is related to charge and T₁ value, lowering the temperature reduces the carrier mobility in the device, resulting in the relative decreasing of charge concentration and the weakening of TQA. Lowering the temperature reduces the quenching of thermal phonons and increases the T₁ value while extending its lifetime, resulting in the enhancement of triplet-triplet annihilation (TTA). At low temperatures, the high magnetic field shape of the MEL changes from slowly increasing to rapidly decreasing. Therefore, the T₁ value can be regulated by varying the current strength and temperature, which further affects the strength of ISC, TQA and TTA, and the luminescence and efficiency of the device can be effectively improved by reducing TQA and ISC. This work is of great significance in understanding the luminescence mechanism of small molecule tandem devices and studying the mechanism for improving their photovoltaic properties.

Keywords:

tandem organic electroluminescent device /
interconnect layer /
intersystem crossing /
triplet-charge annihilation

Authors and contacts

Chongqing Key Laboratory of Optoelectronic Functional Materials, College of Physics and Electronic Engineering, Chongqing Normal University, Chongqing 401331, 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 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 器件A和器件B的结构及其电流密度-亮度-发光效率特性　(a) 器件结构图以及Alq₃, HAT-CN的分子结构; (b) 电压-亮度曲线, 插图为电压-电流密度曲线; (c) 电流密度-亮度曲线以及在亮度为1000 cd/m²和15000 cd/m²的色坐标插图; (d) 电流密度-发光效率曲线

Figure 1. Structural diagram of device A and device B and their current density-luminance-luminance efficiency curves: (a) Structural diagrams and molecular structures of Alq₃ and HAT-CN; (b) voltage-luminance curves, insets shows the voltage-current density curves; (c) current density-luminance curves and color coordinate insets at luminance of 1000 cd/m² and 15000 cd/m²; (d) current density-luminance efficiency curves.

DownLoad: Full-Size Img PowerPoint

图 2 不同连接层(无连接层, Alq₃, HAT-CN, Alq₃/HAT-CN, Al/Alq₃/HAT-CN, Alq₃/HAT-CN/TAPC)的器件C—H能级结构图, 其单位为电子伏特(eV)

Figure 2. Energy level structure of device C—H with differ interconnect layer (without interconnect layer, Alq₃, HAT-CN, Alq₃/HAT-CN, Al/Alq₃/HAT-CN, Alq₃/HAT-CN/TAPC), unit is electron volts (eV).

DownLoad: Full-Size Img PowerPoint

图 3 不同连接层的叠层OLED器件C—H (无连接层, HAT-CN, Alq₃/HAT-CN, Al/Alq₃/HAT-CN和Alq₃ /HAT-CN/TAPC)的光电性能　(a) 电压-电流密度曲线; (b) 电压-亮度曲线; (c) 电流密度-亮度曲线; (d) 电流密度-发光效率曲线; (e) 归一化EL光谱图; (f) 器件C—H电压-电流密度双对数曲线图(黑色为拟合曲线)

Figure 3. Optoelectronic properties of tandem OLED devices C—H (without interconnect layer, HAT-CN, Alq₃/HAT-CN, Al/Alq₃/HAT-CN and Alq₃/HAT-CN/TAPC) with different interconnect layers: (a) Voltage-current density curves; (b) voltage-luminance curves; (c) current density-luminance curves; (d) current density-luminance efficiency curves; (e) normalized EL spectra; (f) the double logarithmic curves of voltage-current density of device C—H (black for fitting curve).

DownLoad: Full-Size Img PowerPoint

图 4 单发光单元器件A和叠层OLED器件B在不同电流下的MEL, MC曲线　(a) 器件A的MEL; (b) 器件B的MEL; (c) MEL的低场和高场效应; (d) 器件A的MC; (e) 器件B的MC; (f) MC的低场和高场效应

Figure 4. The MEL, MC curves of single EL unit device A and tandem OLED device B at different current: (a) MEL curves of device A; (b) MEL curves of device B; (c) MEL_LFE and MEL_HFE; (d) MC curves of device A; (e) MC curves of device B; (f) MC_LFE and MC_HFE.

DownLoad: Full-Size Img PowerPoint

图 5 室温下不同连接层叠层OLED器件D, F—H(Alq₃, Alq₃/HAT-CN, Al/Alq₃/HAT-CN和Alq₃/HAT-CN/TAPC)的MEL和MC曲线, 以及MEL的低场效应和高场效应随电流的变化　(a) MEL曲线; (b) MC曲线; (c) 随电流变化的MEL低场效应; (d) 随电流变化的MEL高场效应

Figure 5. The MEL and MC curves of different interconnect layer tandem OLED devices D, F–H (Alq₃, Alq₃/HAT-CN, Al/Alq₃/HAT-CN and Alq₃/HAT-CN/TAPC) at room temperature, and the variation of MEL_LFE and MEL_HFE with current: (a) MEL curves; (b) MC curves; (c) MEL_LFE of the current variation; (d) MEL_HFE of the current variation.

DownLoad: Full-Size Img PowerPoint

图 6 在一定电流下随温度变化的Alq₃/HATCN连接层叠层OLED的MEL和MC曲线　(a) 100 μA的MEL; (b) 800 μA的MEL; (c) 100 μA的MC; (d) 800 μA的MC

Figure 6. The MEL and MC curves of Alq₃/HATCN interconnect layer tandem OLED that vary with temperature under a certain current: (a) MEL curves of 100 μA; (b) MEL curves of 800 μA; (c) MC curves of 100 μA; (d) MC curves of 800 μA.

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图 7 (a) 单发光单元OLED能级图, 其单位为电子伏特(eV); (b) Alq₃发光材料器件的机制形成过程图

Figure 7. (a) Energy level structure of single EL unit OLED, unit is electron volts (eV); (b) mechanisms formation process involved in Alq₃ luminescent material devices.

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表 1 单发光单元器件A和连接层为Alq₃/HAT-CN叠层器件B, 以及不同连接层的叠层器件C—H的光电性能

Table 1. Photovoltaic performance of single EL unit device A, tandem device B with Alq₃/HAT-CN as the interconnect layers, and tandem devices C—H with different interconnect layers.

Device	Voltage_on/V	Voltage/V	Luminance/(cd·m^–2)		Luminance efficiency/(cd·A^–1)
Device	Voltage_on/V	J₈₀	Max	J₈₀	Max	J₈₀
A	4.09	7.96	36640	4007.14	5.53	5.00
B	7.65	17.45	21710	10410.00	13.28	12.92
C	4.05	11.73	15200	3353.27	5.29	4.19
D	9.38	18.39	12080	5494.57	9.00	6.84
E	5.43	17.94	9181	3072.57	4.23	3.84
F	7.89	15.32	26420	11189.86	15.35	13.85
G	8.25	18.20	14530	6039.05	8.79	7.54
H	6.76	12.54	13630	6340.97	8.22	7.91
注: J表示电流密度, J₈₀数据列代表电流密度为80 mA·cm^–2时, 相应参量的取值; Max数据列表示相应参量的最大值.

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[2]	Chen Q S, Jia W Y, Chen L X, Yuan D, Zou Y, Xiong Z H 2016 Sci. Rep. 6 25331 Google Scholar
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[20]	Wang Y, Ning Y R, Wu F J, Chen J, Chen X L, Xiong Z H 2022 Adv. Funct. Mater. 32 2202882 Google Scholar
[21]	Zhang T T, Holford D F, Gu H, Kreouzis T, Zhang S J, Gillin W P 2016 Appl. Phys. Lett. 108 023303 Google Scholar
[22]	Van Reenen S, Kersten S P, Wouters S H W, et al. 2013 Phys. Rev. B 88 125203 Google Scholar
[23]	Chang Q, Lü Z Y, Yin Y H, Xiao J, Wang J L 2022 Displays 75 102306 Google Scholar
[24]	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 物理学报 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
[25]	Keawin T, Prachumrak N, Namuangruk S, et al. 2015 RSC Adv. 5 73481 Google Scholar
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[27]	Can M, Havare A K, Aydın H, Yagmurcukardes N, Demic S, Icli S, Okur S 2014 Appl. Surf. Sci. 314 1082 Google Scholar
[28]	Talik N A, Yeoh K H, Ng C Y B, Tan C Y, Yap B K 2016 J. Lumin. 169 61 Google Scholar
[29]	Yuan P S, Guo X M, Qiao X F, Yan D H, Ma D G 2019 Adv. Opt. Mater. 7 1801648 Google Scholar
[30]	Engmann S, Bittle E G, Richter L J, Hallani R K, Anthony J E, Gundlach D J 2021 J. Mater. Chem. C 9 10052 Google Scholar
[31]	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
[32]	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
[33]	邓金秋, 汤仙童, 潘睿亨, 胡叶倩, 朱洪强, 熊祖洪, 陈晓莉 2018 科学通报 63 2974 Google Scholar Deng J Q, Tang X T, Pan R H, Hu Y Q, Zhu H Q, Xiong Z H, Chen X L 2018 Chin. Sci. Bull. 63 2974 Google Scholar
[34]	Jou J H, Lin W J, Shih S H, Wang Y S, Sahoo S, Singh M, Tsai Y C, Wen S W 2023 Electronics 12 2099 Google Scholar
[35]	Chen P, Peng Q M, Yao L, Gao Na, Li F 2013 Appl. Phys. Lett. 102 063301
[36]	Peng Q M, Li A W, Fan Y X, Chen P, Li F 2014 J. Mater. Chem. C 2 6264 Google Scholar
[37]	Liu H, Jia W Y, Zhang Y, Zhang Q M, Lei Y L, Lu C L, Ling Y Z, Xiong Z H 2014 Synth. Met. 198 6 Google Scholar
[38]	Desai P, Shakya P, Kreouzis T, Gilin W P, Morley N A, Gibbs M R J 2007 Phys. Rev. B 75 094423 Google Scholar
[39]	Sheng Y, Nguyen T D, Veeraraghavan G, Mermer Ö, Wohlgenannt M, Qiu S, Scherf U 2006 Phys. Rev. B 74 045213 Google Scholar
[40]	Baniya S, Pang Z Y, Sun D L, Zhai Y X, Kwon O, Choi H, Choi B, Lee S, Vardeny Z V 2016 Adv. Funct. Mater. 26 6930 Google Scholar
[41]	Janssen P, Cox M, Wouters S H W, Kemerink M, Wienk M M, Koopmans B 2013 Nat. Commun. 4 2286 Google Scholar
[42]	Kim C Y, Lee C, Kim H J, Hwang J, Godumala M, Jeong J E, Woo H Y, Cho M J, Park S, Choi D H 2020 J. Mater. Chem. C 8 6780 Google Scholar
[43]	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
[44]	Yuan P S, Qiao X F, Yan D H, Ma D G 2018 J. Mater. Chem. C 6 5721 Google Scholar
[45]	Shao M, Yan L, Li M X, Ilia L, Hu B 2013 J. Mater. Chem. C 1 1330 Google Scholar

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Vol. 72, Issue 21 - 2023-11-05

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Exciton regulation mechanism of Alq₃/HAT-CN tandem electroluminescent devices

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

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Exciton regulation mechanism of Alq3/HAT-CN tandem electroluminescent devices

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

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Exciton regulation mechanism of Alq₃/HAT-CN tandem electroluminescent devices