Perovskite light-emitting diodes based on solution-processed metal-doped nickel oxide hole injection layer

Wu Jia-Long; Dou Yong-Jiang; Zhang Jian-Feng; Wang Hao-Ran; Yang Xu-Yong

doi:10.7498/aps.69.20191269

Abstract

Formamidinium lead bromide (FAPbBr₃) perovskite nanocrystals (NCs) have attracted great attention due to their remarkable performances of low cost, high color purity and tunable band gap. However, in a typical FAPbBr₃ perovskite light-emitting diode(LED), PEDOT:PSS, with hygroscopic and acidic nature, serves as a hole injection layer (HIL), thus leading to the device stability to decrease seriously. Device stability is one critical issue that needs improving for future applications. Here in this study, the nickel oxide (NiO) film prepared by the solution method is adopted as the HIL of the FAPbBr₃ perovskite LED to substitute detrimental PEDOT:PSS. Compared with the control device with PEDOT:PSS HIL, the resulting LED based on NiO film has the operating lifetime twice as great as that based on the PEDOT:PSS film. For further enhancing the performance of FAPbBr₃ LED, two metal dopants (Cs and Li) are introduced to improve the hole injection capability of NiO film and the charge carriers’ balance of device. With Hall measurements, both NiO and Cs/Li-doped NiO demonstrate a full p-type semiconductor characteristic. Increasing the doping concentration in the film can increase the carrier concentration and reduce the carrier mobility. This decreased carrier mobility results from the increased scattering due to grain boundaries and impurity phases, seriously at high Cs/Li concentration. As a result, the device, based on the NiO film (doping 2 mol% Cs) shows the best performance with a maximum brightness value of 2970 cd/m², current efficiency of 43 cd/A and external quantum efficiency (EQE) of 11.0%, thus its efficiency is increased nearly by twice compared with that of the PEDOT:PSS-based device. The results pave the way for making highly efficient and stability perovskite LEDs based on FAPbBr₃ NCs.

Keywords:

formamidinium lead bromide perovskite nanocrystals /
nickel oxide /
metal dopants /
light emitting diodes

Authors and contacts

1.
Shanghai University Microelectronic R&D Center, Shanghai University, Shanghai 201900, China
2.
Key Laboratory of Advanced Display and System Applications, Ministry of Education, Shanghai University, Shanghai 200040, China

Corresponding author: Yang Xu-Yong, yangxy@shu.edu.cn

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2016YFB0401702), the National Natural Science Foundation of China (Grant Nos. 51675322, 61605109, 61735004), the Shanghai Rising-Star Program, China (Grant No. 17QA1401600), and the Program for Professors of Special Appointment (Eastern Scholar) of the Higher Education Institutions of Shanghai, China.

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References

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Cited By

图 1 (a) 器件结构示意图; (b) 器件横断面SEM截面图; (c) 能级结构示意图; (d) FAPbBr₃ NCs的XRD图谱(插图为其TEM图)

Figure 1. (a) Device structure; (b) cross-sectional SEM image of the device; (c) energy band diagram; (d) XRD diffraction pattern of the FAPbBr₃ NCs (inset: TEM image of the FAPbBr₃ NCs).

DownLoad: Full-Size Img PowerPoint

图 2 (a) 器件的归一化电致发光和光致发光光谱; PEDOT:PSS和NiO空穴注入层器件的(b) 电流密度-电压曲线, (c) 亮度-电压曲线和(d)电流密度-外量子效率-电压特性

Figure 2. (a) Normalized electroluminescence and photoluminescence spectra of the device; (b) J-V characteristics, (c) L-V characteristics, and (d) CE-EQE-V characteristics of the PEDOT:PSS- and NiO-based device.

DownLoad: Full-Size Img PowerPoint

图 3 PEDOT:PSS和NiO空穴注入层的器件寿命特性图

Figure 3. Operating lifetime characteristics of the PEDOT:PSS and NiO-based devices.

DownLoad: Full-Size Img PowerPoint

图 4 掺杂不同浓度(2, 4, 6 mol%)Cs的NiO器件的(a) 电流密度-亮度-电压特性和(b)电流效率-外量子效率-电压特性; 掺杂不同浓度(2, 4, 6 mol%)Li的NiO器件的(c) 电流密度-亮度-电压特性和(d)电流效率-外量子效率-电压特性

Figure 4. (a) J-L-V characteristics of the devices with Cs: NiO; (b) CE-EQE-V characteristics of the devices with Cs: NiO; (c) J-L-V characteristics of the devices with Li: NiO; (d) CE-EQE-V characteristics of the devices with Li: NiO at different concentrations (2, 4 and 6 mol%).

DownLoad: Full-Size Img PowerPoint

表 1 金属掺杂NiO的器件性能

Table 1. The performance of devices with metal-doped NiO.

金属掺杂浓度	V_on/V ^a	L_max/ cd·m^–2 ^b	CE/ cd·A^–1 ^c	EQE/% ^d
2 mol% Cs	3	2970	43.0	11.0
4 mol% Cs	3	2610	27.8	7.1
6 mol% Cs	3	2090	8.7	2.2
2 mol% Li	3	2500	32.3	8.3
4 mol% Li	3	3490	41.8	10.7
6 mol% Li	3	2950	16.0	4.1
^a开启电压, 亮度为1 cd·m^–2 时的电压; ^b最高的亮度; ^c最高的电流效率; ^d最高的外量子效率.

DownLoad: CSV

表 2 Cs掺杂NiO薄膜的电学性能

Table 2. Electrical properties of Cs-doped NiO films.

金属掺杂浓度	ρ/Ω·cm ^a	μ/cm²·V^–1·s^–1 ^b	p/cm^–3 ^c
0	2.6 × 10^–1	1.7	2.1 × 10¹⁸
2 mol% Cs	1.8 × 10^–1	1.5	5.3 × 10¹⁸
4 mol% Cs	1.7 × 10^–1	0.5	6.0 × 10¹⁸
6 mol% Cs	1.4 × 10^–1	0.2	7.4 × 10¹⁸
2 mol% Li	2.2 × 10^–1	1.3	4.6 × 10¹⁸
4 mol% Li	1.8 × 10^–1	1.1	5.7 × 10¹⁸
6 mol% Li	1.5 × 10^–1	0.3	6.9 × 10¹⁸
^a电阻率; ^b迁移率; ^c载流子浓度(空穴).

DownLoad: CSV

[1]	Cho H, Jeong S H, Park M H, Kim Y H, Wolf C, Lee C L, Heo J H, Sadhanala A, Myoung N, Yoo S, Im S H, Friend R H, Lee T W 2015 Science 350 1222 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]	Yuan M, Quan L N, Comin R, Walters G, Sabatini R, Voznyy O, Hoogland S, Zhao Y, Beauregard E M, Kanjanaboos P, Lu Z, Kim D H, Sargent E H 2016 Nat. Nanotechnol. 11 872 Google Scholar
[4]	Xiao Z, Kerner R A, Zhao L, Tran N L, Lee K M, Koh T W, Scholes G D, Rand B P 2017 Nat. Photonics 11 108 Google Scholar
[5]	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
[6]	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
[7]	Fu Y, Zhu H, Schrader A W, Liang D, Ding Q, Joshi P, Hwang L, Zhu X Y, Jin S 2016 Nano Lett. 16 1000 Google Scholar
[8]	Manser J S, Christians J A, Kamat P V 2016 Chem. Rev. 116 12956 Google Scholar
[9]	Protesescu L, Yakunin S, Bodnarchuk M I, Bertolotti F, Masciocchi N, Guagliardi A, Kovalenko M V 2016 J. Am. Chem. Soc. 138 14202 Google Scholar
[10]	Song J, Hu W, Wang X F, Chen G, Tian W, Miyasaka T J 2016 Mater. Chem. A 4 8435 Google Scholar
[11]	Smecca E, Numata Y, Deretzis I, Pellegrino G, Boninelli S, Miyasaka T, LaMagna A, Alberti A 2016 Phys. Chem. Chem. Phys. 18 13413 Google Scholar
[12]	Perumal A, Shendre S, Li M, Tay Y K E, Sharma V K, Chen S, Wei Z, Liu Q, Gao Y, Buenconsejo P J S, Tan S T, Gan C L, Xiong Q, Sum T C, Demir H V 2016 Sci. Rep. 6 36733 Google Scholar
[13]	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
[14]	Cui J, Meng F P, Zhang H, Cao K, Yuan H, Cheng Y, Huang F, Wang M K 2014 ACS Appl. Mater. Interfaces 6 22862 Google Scholar
[15]	Cao F, Wang H, Shen P, Li X, Zheng Y, Shang Y Q, Zhang J H, Ning Z, Yang X 2017 Adv. Funct. Mater. 27 1704278 Google Scholar
[16]	Chih Y, Wang J, Yang R, Liu C, Chang Y, Fu Y, Lai W, Chen P, Wen T, Huang Y, Tsao C, Guo T 2016 Adv. Mater. 28 8687 Google Scholar
[17]	Wang Z, Luo Z, Zhao C, Guo Q, Wang Y, Wang F, Bian X, Alsaedi A, Hayat T, Tan Z 2017 J. Phys. Chem. C 121 28132 Google Scholar
[18]	Lee S, Kim D B, Hamilton L, Daboczi M, Nam Y S, Lee B R, Zhao B, Jang C H, Friend R, Kim J, Song M H 2018 Adv. Sci. 5 1801350 Google Scholar
[19]	Wang H, Zhang X, Wu Q, Cao F, Yang D, Shang Y, Ning Z, Zhang W, Zheng W, Yan Y, Kershaw S V, Zhang L, Rogach A L, Yang X 2019 Nat. Commun. 10 665 Google Scholar
[20]	Wang H, Li X, Yuan M, Yang X 2018 Small 14 1703410 Google Scholar
[21]	Levchun L, OsvetA, Tang X F 2017 Nano Lett. 17 2765
[22]	Empedocles S A, Bawendi M G 1997 Science 278 2114 Google Scholar
[23]	Mashford B S, Stevenson M, Popvic Z, Hamilton C, Zhou Z, Breen C, Steckel J, Bulovic V, Bawendi M, Coe-Sullivan S, Kazlas P T 2013 Nat. Photonics 7 407 Google Scholar
[24]	Park S Y, Kim H R, Kang Y J, Kim D H, Kang J W 2010 Sol. Energy Mater. Sol. Cells 94 2332 Google Scholar
[25]	Yang Y X, Zheng Y, Cao W R, Titov A, Hyvonen J, Manders J R, Xue J G, Holloway P H, Qian L 2015 Nat. Photonics 9 259 Google Scholar
[26]	Dai X, Zhang Z, Jin Y, Niu Y, Cao H, Liang X, Chen L, Wang J, Peng X 2014 Nature 515 96 Google Scholar
[27]	Kim H P, Kim J, Kim B S, Kim H M, Kim J, Yusoff A R B M, Jang J, Nazeeruddin M K 2017 Adv. Opt. Mater. 5 1600920 Google Scholar
[28]	Fu F, Feurer T, Weiss T P, Pisoni S, Avancini E, Andres C, Buecheler S, Tiwari A N 2016 Nat. Energy 2 16190
[29]	Shi Z, Li Y, Zhang Y, Chen Y, Li X, Wu D, Xu T, Shan C, Du G 2017 Nano Lett. 17 313 Google Scholar
[30]	Shi Z, Li S, Li Y, Ji H, Li X, Wu D, Xu T, Chen Y, Tian Y, Zhang Y, Shan C, Du G 2018 ACS Nano 12 1462 Google Scholar
[31]	Alidoust N, Carter E A 2015 Phys. Chem. Chem. Phys. 17 18098 Google Scholar
[32]	Kim J H, Liang P W, Williams S T, Cho N, Chueh C C, Glaz M S, Ginger D S, Jen A K Y 2015 Adv. Mater. 27 695 Google Scholar
[33]	Zhang J, Cai G, Zhou D, Tang H, Wang X, Gu C, Tu J 2014 J. Mater. Chem. C 2 7013 Google Scholar
[34]	Popescu I, Skoufa Z, Heracleous E, Lemonidou A, Marcu I C 2015 Phys. Chem. Chem. Phys. 17 8138 Google Scholar
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[36]	Chen S C, Kuo T Y, Lin Y C, Lin H C 2011 Thin Solid Films 519 4944 Google Scholar
[37]	Hwang J D, Ho T H 2017 Mater. Sci. Semicond. Process. 71 396 Google Scholar
[38]	Chen W, Wu Y, Fan J, Djurišic A B, Liu F, Tam H W, Ng A, Surya C, Chan W K, Wang D, He Z B 2018 Adv. Energy Mater. 8 1703519 Google Scholar

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