High efficiency green perovskite light-emitting diodes based on exciton blocking layer

Wang Run; Jia Ya-Lan; Zhang Yue; Ma Xing-Juan; Xu Qiang; Zhu Zhi-Xin; Deng Yan-Hong; Xiong Zu-Hong; Gao Chun-Hong

doi:10.7498/aps.69.20191263

Abstract

In recent years, metal halide perovskite materials, owing to their excellent photoelectric properties including high photoluminescence quantum yield, high color purity, tunable band gap, etc., have been regarded as new-generation lighting sources and are widely used to fabricate perovskite light-emitting diodes (PeLEDs). Though great progresses have been made in recent years, neither the efficiency nor stability has not yet reached the requirements of commercialization. Thus, further improvement is needed. In this work, a small organic molecule material, namely 4,4'-cyclohexylidenebis[N,N-bis(p-tolyl)aniline] (TAPC) with a wide bandgap and a good hole transport ability, is used as an exciton blocking layer by utilizing the spin-coating method to improve the stability and efficiency of PeLEDs. Highly efficient and stable CsPbBr₃ PeLEDs are finally realized. The physical mechanism related to the improved electroluminescence performance is investigated thoroughly. Firstly, the stepped energy level alignment is formed, since the highest occupied molecular orbital energy level (HOMO) of TAPC is located between the HOMO of (3,4-ethylenedioxythiophene):poly(p-styrene sulfonate) (PEDOT: PSS) and the valence band of CsPbBr₃, which is beneficial to hole injection and transport. Meanwhile, the lowest unoccupied molecular orbital level of TAPC is high enough to prevent electrons from leaking into the anode effectively and confine electrons and excitons well in the emitting layer. Secondly, the introduction of the TAPC layer can avoid the direct contact between the perovskite light emitting layer and the strong acidic layer of PEDOT:PSS, thereby eliminating the related excitons quenching, which can further increase the radiative recombination.

Keywords:

Authors and contacts

1.
School of Physical Science and Technology, Southwest University, Chongqing 400715, China
2.
Applied Basic Research Base of Optoelectronic Information Technology of Hunan Province, Hengyang Normal University, Hengyang 421002, China

Corresponding author: Gao Chun-Hong, gch0122@swu.edu.cn

Funds: Project supported by the Postgraduate Science Research Innovation Program of Chongqing, China (Grant No. CYS190950), the Open Fund of Applied Basic Research Base of Optoelectronic Information Technology of Hunan Province, China (Grant No. GD19K01), the Fundamental Research Funds for the Central Universities (Grant No. XDJK2018C082), the Special Program for Talent Training in West China funded by National Study Abroad Fund, China (Grant No. [2018]10006), the Innovation and Entrepreneurship Training Program for College Students of Southwest University, China (Grant No. X201910635332), the Young Scientists Fund of the Natural Science Foundation of Hunan Province, China (Grant No. 2018JJ3010), and the Program for Excellent Talents of Hengyang Normal University, China

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References

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Cited By

图 1 (a) PeLEDs的器件结构; (b) PeLEDs的能级图

Figure 1. (a) Device structure of PeLEDs; (b) schematic energy level diagram of PeLEDs.

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图 2 PeLEDs的EL性能表征　(a)电流密度-电压; (b)亮度-电压; (c)电流效率-电压-外量子效率; (d) PeLEDs (TAPC浓度为5 mg/mL)在不同电压下的EL光谱, 内插图是不同TAPC浓度的PeLEDs在电压为5 V时的归一化EL谱

Figure 2. EL performance of PeLEDs: (a) Current density-voltage (J-V); (b) luminance-voltage (L-V); (c) current-efficiency-voltage-external quantum efficiency (CE-V-EQE); (d) EL spectra of PeLEDs with 5 mg/mL TAPC at different applied voltages; the inset is normalized EL spectra of PeLEDs with different concentrations of TAPC at the same applied voltage of 5 V.

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图 3 PeLEDs的稳定性表征

Figure 3. The EL stability of PeLEDs.

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图 4 (a) ITO/PEDOT:PSS/CsPbBr₃和(b) ITO/PEDOT:PSS/TAPC/CsPbBr₃样品的SEM图; (c) ITO/PEDOT:PSS/CsPbBr₃和(d) ITO/PEDOT:PSS/TAPC/CsPbBr₃样品的CsPbBr₃颗粒尺寸统计分布

Figure 4. SEM images of (a) ITO/PEDOT:PSS/CsPbBr₃ and (b) ITO/PEDOT:PSS/TAPC/CsPbBr₃; the size distribution of CsPbBr₃ grain on (c) ITO/PEDOT:PSS/CsPbBr₃ and (d) ITO/PEDOT:PSS/TAPC/CsPbBr₃.

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图 5 在PEDOT:PSS和PEDOT:PSS/TAPC衬底上的CsPbBr₃薄膜的表征　(a)晶体结构(XRD); (b)紫外吸收, 内插图是在500−518 nm波长范围吸收的放大图; (c) PL光谱, 内插图是在520−535 nm波长范围PL的放大图; (d) TRPL曲线

Figure 5. Characteristics of CsPbBr₃ film on PEDOT:PSS and PEDOT:PSS/TAPC: (a) XRD; (b) absorption, and the inset is a large image of normalized PL spectra from 500 to 518 nm; (c) normalized PL spectra, and the inset is a large image of normalized PL spectra from 520 to 535 nm; (d) TRPL decay curves.

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图 6 单空穴器件的电流密度-电压特性曲线

Figure 6. Current density-voltage characteristics of hole-dominated devices.

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图 7 激子界面复合效应　(a) PEDOT:PSS/CsPbBr₃; (b) PEDOT:PSS/TAPC/CsPbBr₃

Figure 7. Exciton recombination interface effects: (a) PEDOT: PSS/TAPC/CsPbBr₃; (b) PEDOT:PSS/CsPbBr₃.

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表 1 PeLEDs性能

Table 1. List of EL performance of PeLEDs.

器件	TAPC浓度/mg·mL^–1	最大亮度/cd·m^–2	最大电流效率/cd·A^–1	外量子效率/%	色坐标(x, y)
A	0	2396	1.81	0.47	(0.13, 0.80)
B	2	6081	4.52	1.17	(0.13, 0.80)
C	5	13198	6.84	1.77	(0.13, 0.80)
D	8	3678	1.13	0.29	(0.13, 0.80)

DownLoad: CSV

表 2 瞬态荧光寿命参数统计列表

Table 2. List of TRPL parameters.

Films	B₁/%	B₂/%	τ₁/ns	τ₂/ns	τ_ave/ns
PEDOT:PSS/CsPbBr₃	79	21	4.86	210.45	47.44
PEDOT:PSS/TAPC/CsPbBr₃	75	25	5.72	212.65	57.64

DownLoad: CSV

[1]	Abdi-Jalebi M, Andaji-Garmaroudi Z, Cacovich S, Stavrakas C, Philippe B, Richter J M, Alsari M, Booker E P, Hutter E M, Pearson A J, Lilliu S, Savenije T J, Rensmo H, Divitini G, Ducati C, Friend R H, Stranks S D 2018 Nature 555 497 Google Scholar
[2]	Huang H, Raith J, Kershaw S V, Kalytchuk S, Tomanec O, Jing L H, Susha A S, Zboril R, Rogach A L 2017 Nat. Commun. 8 996 Google Scholar
[3]	Wang H R, Zhang X, Wu Q Q, Cao F, Yang D W, Shang Y Q, Ning Z J, Zhang W, Zheng W T, Yan Y F, Kershaw S V, Zhang L J, Rogach A L, Yang X Y 2019 Nat. Commun. 10 665 Google Scholar
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[16]	Brenner P, Stulz M, Kapp D, Abzieher T, Paetzold U W, Quintilla A, Howard I A, Kalt H, Lemmer H 2016 Appl. Phys. Lett. 109 141106 Google Scholar
[17]	Wang Y C, Li H, Hong Y H, Hong K B, Chen F C, Hsu C H, Lee R K, Conti C, Kao T S, Lu T C 2019 ACS Nano 13 5421 Google Scholar
[18]	Ji L, Hsu H Y, Lee J C, Bard A J, Yu E T 2018 Nano Lett. 18 994 Google Scholar
[19]	Tian C C, Wang F, Wang Y P, Yang Z, Chen X J, Mei J J, Liu H Z, Zhao D X 2019 ACS Appl. Mater. Interfaces 11 15804 Google Scholar
[20]	Han D B, Imran M, Zhang M J, Chang S, Wu X G, Zhang X, Tang J L, Wang M S, Ali S S, Li X G, Yu G, Han J B, Wang L X, Zou B S, Zhong H Z 2018 ACS Nano 12 8808 Google Scholar
[21]	Gao C H, Yu F X, Xiong Z Y, Dong Y J, Ma X J, Zhang Y, Jia Y L, Wang R, Chen P, Zhou D Y, Xiong Z H 2019 Org. Electron. 70 264 Google Scholar
[22]	Zhao L F, Lee K M, Roh K D, Khan S U Z, Rand B P 2019 Adv. Mater. 31 1805836 Google Scholar
[23]	Braly I L, deQuilettes D W, Pazos-Outón L M, Burke S, Ziffer M E, Ginger D S, Hillhouse H W 2018 Nat. Photon. 12 355 Google Scholar
[24]	Zhang X, Xu B, Zhang J B, Gao Y, Zheng Y J, Wang K, Sun X W 2016 Adv. Funct. Mater. 26 4595 Google Scholar
[25]	Gangishetty M K, Sanders S N, Congreve D N 2019 ACS Photonics 6 1111 Google Scholar
[26]	Zhang X L, Liu H, Wang W G, Zhang J B, Xu B, Karen K L, Zheng Y J, Liu S, Cheng S M, Wang K, Sun X W 2017 Adv. Mater. 29 1606405 Google Scholar
[27]	Chen P, Xiong Z Y, Wu X Y, Shao M, Ma X J, Xiong Z H, Gao C H 2017 J. Phys. Chem. Lett. 8 1810 Google Scholar
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[29]	段聪聪, 程露, 殷垚, 朱琳 2019 物理学报 68 158503 Google Scholar Duan C C, Chen L, Yin Y, Zhu L 2019 Acta Phys. Sin. 68 158503 Google Scholar
[30]	瞿子涵, 储泽马, 张兴旺, 游经碧 2019 物理学报 68 158504 Google Scholar Qu Z H, Chen Z M, Zhang X W, You J B 2019 Acta Phys. Sin. 68 158504 Google Scholar
[31]	黎振超, 陈梓铭, 邹广锐兴, 叶轩立, 曹镛 2019 物理学报 68 158505 Google Scholar Li Z C, Chen Z M, Zou G R X, Yip H L, Cao Y 2019 Acta Phys. Sin. 68 158505 Google Scholar
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[35]	Peng X F, Wu X Y, Ji X X, Ren J, Wang Q, Li G Q, Yang X H 2017 J. Phys. Chem. Lett. 8 4691 Google Scholar
[36]	Wang Z J, Li Z R, Zhou D L, Yu J S 2017 Appl. Phys. Lett. 111 233304 Google Scholar
[37]	Lin C Y, Chen P, Xiong Z Y, Liu D B, Wang G, Meng Y, Song Q L 2018 Nanotechnology 29 075203 Google Scholar
[38]	Zou Y T, Ban M Y, Yang Y G, Bai S, Wu C, Han Y J, Wu T, Tan Y S, Huang Q, Gao X Y, Song T, Zhao Q, Sun B Q 2018 ACS Appl. Mater. Interfaces 10 24320 Google Scholar
[39]	Meng Y, Ahmadi M, Wu X Y, Xu T F, Xu L, Xiong Z H, Chen P 2019 Org. Electron. 64 47 Google Scholar
[40]	Kim S Y, Jeong W, Mayr C, Park Y S, Kim K H, Lee J H, Moon C K 2013 Adv. Funct. Mater. 23 3896 Google Scholar
[41]	Cui L S, Liu Y, Yuan X D, Li Q, Jiang Z Q, Liao L S 2013 J. Mater. Chem. C 1 8177 Google Scholar
[42]	Yu F X, Zhang Y, Xiong Z Y, Ma X J, Chen P, Xiong Z H, Gao C H 2017 Org. Electron. 50 480 Google Scholar
[43]	Yuan M J, Quan L N, Comin R, Walters G, Sabatini R, Voznyy O, Hoogland S, Zhao Y B, Beauregard E M, Kanjanaboos P, Lu Z H, Kim D H, Sargent E H 2016 Nat. Nanotechnol. 11 872 Google Scholar
[44]	Ban M Y, Zou Y T, Pivett J P.H., Yang Y G, Thomas T H, Tan Y, Song T, Gao X Y, Credington D, Deschler F, Sirringhaus H, Sun B Q 2018 Nat. Commun. 9 3892 Google Scholar
[45]	Dai X L, Deng Y Z, Peng X G, Jin Y Z 2017 Adv. Mater. 29 1607022 Google Scholar
[46]	Wu T, Yang Y G, Zou Y T, Wang Y S, Wu C, Han Y J, Song T, Zhang Q, Gao X Y, Sun B Q 2018 Nanoscale 10 19322 Google Scholar
[47]	Kim Y H, Wolf C, Kim Y T, Cho H C, Kwon W S, Do S G, Sadhanala A, Park C G, Rhee S W, Im S H, Friend H F, Lee T W 2017 ACS Nano 11 6586 Google Scholar
[48]	Zheng K B, Zidek K, Abdellah M, Messing M E, Al-Marri M J, Pullerits T 2016 J. Phys. Chem. C 120 3077
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Vol. 69, Issue 3 - 2020-02-05

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