高效绿光钙钛矿发光二极管研究进展

瞿子涵; 储泽马; 张兴旺; 游经碧

doi:10.7498/aps.68.20190647

摘要

钙钛矿发光二极管具有发光效率高、色纯、发光波长在可见光区间连续可调等优点, 近来成为研究前沿热点. 作为人眼最为敏感的波段, 绿光发射的钙钛矿发光二极管对于白光照明和平板显示具有重要意义, 得到了科研人员的广泛关注. 本文主要介绍绿光钙钛矿发光二极管的发展历史、钙钛矿材料和发光二极管器件的基本结构以及提升绿光钙钛矿发光二极管效率的主要方法. 最后本文对未来绿光钙钛矿发光二极管可能的发展方向进行了简要的预测, 以期对未来该领域的研究提供一些思路.

关键词:

钙钛矿 /
发光二极管 /
绿光 /
效率

Abstract

Perovskite light emitting diodes exhibit the advantages of high color purity, tunable wavelength and low producing cost. Considering these superiorities, one regards perovskite light emitting diodes as very promising candidates for solid state lighting and panel displaying. Human eyes are very sensitive to green light, thus green perovskite light emitting diodes receive the most attention from researchers. Since the advent of the very first green perovskite light emitting diode, the external quantum efficiency has climbed from only 0.1% to over 20%. In this review, we mainly discuss the history of green perovskite light emitting diodes, the basic concepts of perovskite materials and green perovskite light emitting diodes, and the common methods to improve the efficiency of green perovskite light emitting diodes. The bandgap of bromide perovskite is about 2.3 eV, which is located just on a green light wavelength scale and thus becomes the suitable emitting layer material for green emission. There are mainly two types of device structures, i.e. regular format and inverted format. The whole working process of green perovskite light emitting diodes can be divided into two stages, i.e. the injection and recombination of charge carriers. One engineers the energy levels of different layers to improve the injection of charge carriers. They also raise up the strategy so-called surface passivation to reduce the defect density at the interface in order to avoid the quenching phenomenon. One usually inserts a buffering layer to realize the surface passivation. Besides, perovskites possess very small exciton binding energy, which is at the same order of magnitudes as the kinetic energy at room temperature. Charge carriers become free in this case, which will severely reduce the radiation recombination probability due to the non-radiation recombination process such as Shockley-Read-Hall effect and Auger recombination. To solve the problem, people fabricate three types of perovskites, namely quasi two-dimensional perovskite, perovskite quantum dot, and perovskite nanocrystal. In this way, the charge carriers can be confined into a limited space and the exciton binding energy will hence be improved. From the efficiency perspective, the green perovskite light emitting diodes promise to be commercialized. However, another critical issue impeding the development of green perovskite light emitting diodes is the stability problem. Comparing with the organic light emitting diodes and inorganic quantum dot light emitting diodes, the lifetime of perovskite light emitting diodes is too limited, which is only approximately one hundred hours under normal conditions. The temperature, moisture and light exposure are all factors that influence the stability of perovskite light emitting diodes.

Keywords:

作者及机构信息

1.
中国科学院半导体研究所, 材料科学重点实验室, 北京　100083

2.
中国科学院大学, 材料科学与光电工程中心, 北京　100049

通信作者: 游经碧, jyou@semi.ac.cn

Authors and contacts

1.
Key Laboratory of Semiconductor Materials Science, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China

2.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: You Jing-Bi, jyou@semi.ac.cn

文章全文

参考文献

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施引文献

图 1 GPeLED效率增长趋势

Fig. 1. Increasing trend of GPeLED’s EQE.

下载: 全尺寸图片幻灯片

图 2 钙钛矿发光二极管的典型结构　(a)正置结构; (b)倒置结构

Fig. 2. Typical device structure of PeLED: (a) Regular structure; (b) inverted structure.

下载: 全尺寸图片幻灯片

图 3 钙钛矿材料中电子、空穴的复合机制^[7]

Fig. 3. Recombination mechanisms of electrons and holes in perovskite^[7].

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图 4 结构为ITO/PEDOT:PSS/MAPbBr₃:PIP/F8/Ca/Ag的器件性能　(a) EQE随电流密度的变化; (b)亮度/电流密度随电压的变化^[9]

Fig. 4. Devices based on the ITO/PEDOT:PSS/MAPbBr₃:PIP/F8/Ca/Ag structure: (a) EQE versus current density; (b) luminance/current density versus voltage^[9].

下载: 全尺寸图片幻灯片

图 5 (a)纳米晶钉扎法步骤图示; (b)纳米晶扫描电子显微镜(SEM)图^[11]

Fig. 5. (a) Schematic illustration of NCP processes; (b) SEM image of grains^[11].

下载: 全尺寸图片幻灯片

图 6 (a)钙钛矿量子点TEM图^[32]; (b)量子点PeLED发光峰位的调节^[33]

Fig. 6. (a) TEM graph of perovskite quantum dot^[32]; (b) the gradual change of wavelength from quantum dot PeLED^[33].

下载: 全尺寸图片幻灯片

图 7 准二维钙钛矿中的能量转移过程^[36]

Fig. 7. Energy transfer process in the quasi-2D perovskite^[36]

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图 8 结构为ITO/Buf-HIL/PEA₂MA_m–1Pb_mBr_3m+1/TPBi/LiF/Al的器件性能　(a) CE随电压的变化; (b)亮度随电压的变化^[30]

Fig. 8. Devices based on the ITO/Buf-HIL/PEA₂MA_m–1Pb_mBr_3m+1/TPBi/LiF/Al structure: (a) Current efficiency vs. voltage; (b) luminance vs. voltage^[30].

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图 9 (a) HIL掺杂后的器件能带结构图; (b) HIL掺杂前后器件的电流效率和亮度^[15]

Fig. 9. (a) Energy band diagram after HIL doping; (b) current efficiency and luminance before and after HIL doping^[15].

下载: 全尺寸图片幻灯片

图 10 对PEDOT:PSS改性后的器件能带结构图^[11]

Fig. 10. Energy band diagram of the device after modification to PEDOT:PSS^[11].

下载: 全尺寸图片幻灯片

图 11 (a) TOPO钝化前后的钙钛矿薄膜光致荧光(PL)谱; (b) TOPO钝化前后的钙钛矿荧光寿命^[15]

Fig. 11. (a) Photoluminescence spectrum of perovskite thin film with and without TOPO passivation; (b) fluorescence lifetime of perovskite thin film with and without TOPO passivation^[15].

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表 1 部分高效GPeLED的工作寿命

Table 1. Working lifetime of some high-efficiency GPeLEDs.

文献	器件结构	最大EQE/%	寿命参数(L₀ = 100 cd·m^–2)
[14]	ITO/ZnO/PVP/Pero/CBP/MoO₃/Al	10.43	T₅₀ = 10 min
[41]	ITO/PEDOT:PSS/Pero/TPBi/LiF/Al	12.1	T₅₀ = 135 min
[15]	ITO/PEDOT:PSS/Pero/TOPO/TPBi/LiF/Al	14.36	T₅₀ = 4.8 h
[4]	ITO/PEDOT:PSS/Pero/PMMA/B3PYMPM/LiF/Al	20.3	T₅₀ = 104.56 h

下载: 导出CSV

[1]	Quan L N, de Arquer F P G, Sabatini R P, Sargent E H 2018 Adv. Mater. 30 1801996 Google Scholar
[2]	Tan Z K, Moghaddam R S, Lai M L, Docampo P, Higler R, Deschler F, Price M, Sadhanala A, Pazos L M, Credgington D, Hanusch F, Bein T, Snaith H J, Friend R H 2014 Nat. Nanotechnol. 9 687 Google Scholar
[3]	Cao Y, Wang N N, Tian H, Guo J S, Wei Y Q, Chen H, Miao Y F, Zou W, Pan K, He Y R, Cao H, Ke Y, Xu M M, Wang Y, Yang M, Du K, Fu Z W, Kong D C, Dai D X, Jin Y Z, Li G Q, Li H, Peng Q M, Wang J P, Huang W 2018 Nature 562 249 Google Scholar
[4]	Lin K B, Xing J, Quan L N, de Arquer F P G, Gong X W, Lu J X, Xie L Q, Zhao W J, Zhang D, Yan C Z, Li W Q, Liu X Y, Lu Y, Kirman J, Sargent E H, Xiong Q H, Wei Z H 2018 Nature 562 245 Google Scholar
[5]	Chen C H, Tang C W 2001 Appl. Phys. Lett. 79 3711 Google Scholar
[6]	Dai X L, Deng Y Z, Peng X G, Jin Y Z 2017 Adv. Mater. 29 1607022 Google Scholar
[7]	Kim Y H, Kim J S, Lee T W 2018 Adv. Mater. DOI: 10.1002/adma.201804595
[8]	彭玮婷, 邵双运, 林子钰, 单宏儒, 张洁瑞 2016 光电子·激光 27 1320 Peng W T, Shao S Y, Lin Z Y, Shan H R, Zhang J R 2016 J. Optoelectron. Laser 27 1320
[9]	Li G R, Tan Z K, Di D W, Lai M L, Jiang L, Lim J H W, Friend R H, Greenham N C 2015 Nano Lett. 15 2640 Google Scholar
[10]	Wang J P, Wang N N, Jin Y Z, Si J J, Tan Z K, Du H, Cheng L, Dai X L, Bai S, He H P, Ye Z Z, Lai M L, Friend R H, Huang W 2015 Adv. Mater. 27 2311 Google Scholar
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[13]	Xiao Z G, Kerner R A, Zhao L F, Tran N L, Lee K M, Koh T W, Scholes G D, Rand B P 2017 Nat. Photon. 11 108 Google Scholar
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[17]	Kim Y H, Lee G H, Kim Y T, Wolf C, Yun H J, Kwon W, Park C G, Lee T W 2017 Nano Energy 38 51 Google Scholar
[18]	Noh J H, Im S H, Heo J H, Mandal T N, Seok S I 2013 Nano Lett. 13 1764 Google Scholar
[19]	Mosconi E, Amat A, Nazeeruddin M K, Gratzel M, de Angelis F 2013 J. Phys. Chem. C 117 13902 Google Scholar
[20]	Kitazawa N, Watanabe Y, Nakamura Y 2002 J. Mater. Sci. 37 3585 Google Scholar
[21]	Veldhuis S A, Boix P P, Yantara N, Li M J, Sum T C, Mathews N, Mhaisalkar S G 2016 Adv. Mater. 28 6804 Google Scholar
[22]	Seo H K, Kim H, Lee J, Park M H, Jeong S H, Kim Y H, Kwon S J, Han T H, Yoo S, Lee T W 2017 Adv. Mater. 29 1605587 Google Scholar
[23]	Yan F, Xing J, Xing G C, Quan L, Tan S T, Zhao J X, Su R, Zhang L L, Chen S, Zhao Y W, Huan A, Sargent E H, Xiong Q H, Demir H V 2018 Nano Lett. 18 3157 Google Scholar
[24]	Schulz P, Edri E, Kirmayer S, Hodes G, Cahen D, Kahn A 2014 Energy Environ. Sci. 7 1377 Google Scholar
[25]	Yin W J, Shi T T, Yan Y F 2014 Appl. Phys. Lett. 104 063903 Google Scholar
[26]	Adjokatse S, Fang H H, Loi M A 2017 Mater. Today 20 413 Google Scholar
[27]	Kumar S, Jagielski J, Yakunin S, Rice P, Chiu Y C, Wang M C, Nedelcu G, Kim Y, Lin S C, Santos E J G, Kovalenko M V, Shih C J 2016 ACS Nano 10 9720 Google Scholar
[28]	Tanaka K, Takahashi T, Ban T, Kondo T, Uchida K, Miura N 2003 Solid State Commun. 127 619 Google Scholar
[29]	Meng L, Yao E P, Hong Z R, Chen H J, Sun P Y, Yang Z L, Li G, Yang Y 2017 Adv. Mater. 29 1603826 Google Scholar
[30]	Byun J, Cho H, Wolf C, Jang M, Sadhanala A, Friend R H, Yang H, Lee T W 2016 Adv. Mater. 28 7515 Google Scholar
[31]	Wang Z J, Huai B X, Yang G J, Wu M G, Yu J S 2018 J. Lumin. 204 110 Google Scholar
[32]	Chiba T, Hoshi K, Pu Y J, Takeda Y, Hayashi Y, Ohisa S, Kawata S, Kido J 2017 ACS Appl. Mater. Interfaces 9 18054 Google Scholar
[33]	Protesescu L, Yakunin S, Bodnarchuk M I, Krieg F, Caputo R, Hendon C H, Yang R X, Walsh A, Kovalenko M V 2015 Nano Lett. 15 3692 Google Scholar
[34]	Song J Z, Fang T, Li J H, Xu L M, Zhang F J, Han B N, Shan Q S, Zeng H B 2018 Adv. Mater. 30 1805409 Google Scholar
[35]	Deng W, Xu X Z, Zhang X J, Zhang Y D, Jin X C, Wang L, Lee S T, Jie J S 2016 Adv. Funct. Mater. 26 4797 Google Scholar
[36]	Wang N N, Cheng L, Ge R, Zhang S T, Miao Y F, Zou W, Yi C, Sun Y, Cao Y, Yang R, Wei Y Q, Guo Q, Ke Y, Yu M T, Jin Y Z, Liu Y, Ding Q Q, Di D W, Yang L, Xing G C, Tian H, Jin C H, Gao F, Friend R H, Wang J P, Huang W 2016 Nat. Photon. 10 699 Google Scholar
[37]	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
[38]	Si J J, Liu Y, He Z F, Du H, Du K, Chen D, Li J, Xu M M, Tian H, He H P, Di D W, Ling C Q, Cheng Y C, Wang J P, Jin Y Z 2017 ACS Nano 11 11100 Google Scholar
[39]	Kim Y H, Cho H, Heo J H, Kim T S, Myoung N, Lee C L, Im S H, Lee T W 2015 Adv. Mater. 27 1248 Google Scholar
[40]	Yambem S D, Liao K S, Alley N J, Curran S A 2012 J. Mater. Chem. 22 6894 Google Scholar
[41]	Lee S, Park J H, Nam Y S, Lee B R, Zhao B D, Di Nuzzo D, Jung E D, Jeon H, Kim J Y, Jeong H Y, Friend R H, Song M H 2018 ACS Nano 12 3417 Google Scholar

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