High-efficiency sky blue perovskite light-emitting diodes with ammonium thiocyanate additive

Gao Jiu-Lin; Lian Ya-Jun; Yang Ye; Li Guo-Qing; Yang Xiao-Hui

doi:10.7498/aps.70.20211046

Abstract

Metal halide perovskite light-emitting diodes have attracted much attention due to their excellent characteristics such as low-cost solution-processing, high luminous efficiency and excellent color purity. However, low luminous efficiency and spectrum stability of blue perovskite light-emitting device restrict the further development of perovskite materials in the field of displays and lighting. Here in this work, we study the effects of ammonium thiocyanate (NH₄SCN) addition on the morphology, crystal structure, photo-physics, charge transport and electroluminescence properties of quasi-two-dimensional mixed-halide perovskite films by measuring scanning electron microscope (SEM), X-ray diffraction (XRD), UV-Vis spectrum, steady-state photoluminescence (PL), and transient PL and analyzing the current density–voltage characteristics of hole-dominated device and current density-voltage-luminance plots of light-emitting device. The results indicate that ammonium thiocyanate (NH₄SCN) can effectively passivate the defects, improve the crystallinity, and modulate the phase distribution of quasi-two-dimensional mixed-halide perovskite film, thereby increasing charge transport and luminescent efficiency. Notably, PL intensity of the 20%-NH₄SCN sample is 1.7 times higher than that of the control sample, which is attributed to the defect passivation effect of NH₄SCN probably due to the Lewis acid-base interaction with Pb²⁺. Meanwhile, the hole mobility of the 20%-NH₄SCN sample is measured to be 1.31 × 10^–5 cm²/(V·s), which is much higher than that of the control sample (3.58 × 10^–6 cm²/(V·s)). As a result, sky-blue quasi-two-dimensional mixed-halide perovskite light-emitting diode with 20%-NH₄SCN possesses an EL maximum at 486 nm and a maximum external quantum efficiency (EQE) of 5.83% and a luminance of 1258 cd/m², which are 6.7 and 3.6 times higher than those of the control device without NH₄SCN, respectively. At the same time, the EL spectra of the 20%-NH₄SCN device are barely changed under different operating voltages, whereas the EL spectra of the control device show a 7–10 nm red-shift under the same condition, indicating that the NH₄SCN addition inhibits halide phase separation and improves the EL spectrum stability. In addition, the T₅₀ operational life-time of the 20%-NH₄SCN device is measured to be about 110 s, which is superior to that of the control device (39 s) due to improved film quality of NH₄SCN-modified sample. This research provides a simple and effective method to improve the performances of quasi-two-dimensional mixed-halide perovskite blue-emitting diodes.

Keywords:

quasi-two-dimensional mixed-halide perovskites /
blue-emitting diodes /
ammonium thiocyanate /
defect passivation

Authors and contacts

School of Physical Science and Technology, Southwest University, Chongqing 400715, China

Corresponding author: Yang Xiao-Hui, xhyang@swu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11474232)

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References

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Cited By

图 1 NH₄SCN浓度分别为　(a) 0%; (b) 10%; (c) 20%; (d) 40%准二维钙钛矿薄膜的SEM形貌(插图为高分辨率SEM 图像)和 (e) XRD图谱

Figure 1. Top-view SEM images of the samples with the NH₄SCN concentration of (a) 0%; (b) 10%; (c) 20%; (d) 40% (Insets: high-resolution SEM images); (e) XRD patterns of the samples.

DownLoad: Full-Size Img PowerPoint

图 2 (a) 不同NH₄SCN浓度样品的紫外-可见吸收光谱; (b) 光致发光光谱

Figure 2. (a) UV-Vis absorption spectra; (b) steady-state photoluminescence spectra of the samples with different NH₄SCN concentrations.

DownLoad: Full-Size Img PowerPoint

图 3 (a) 405 nm激光激发下样品的时间分辨光致发光衰减曲线; (b) 空穴主导型器件的电流-电压特性曲线

Figure 3. (a) Time-resolved photoluminescence decay curves of the samples under 405 nm laser excitation; (b) current density-voltage characteristics of hole-dominated devices.

DownLoad: Full-Size Img PowerPoint

图 4 (a) 器件结构示意图; (b) 电流密度-电压-亮度曲线; (c) 外量子效率-电流密度特性

Figure 4. (a) Schematic diagram of device structure; (b) current density-voltage-luminance curves; (c) external quantum efficiency-current density characteristics of the devices with different NH₄SCN concentrations.

DownLoad: Full-Size Img PowerPoint

图 5 (a) 不同NH₄SCN浓度器件的归一化电致发光光谱; (b) 在不同电压下0% NH₄SCN和 (c) 20% NH₄SCN器件电致发光光谱, 插图给出20% NH₄SCN器件的照片; (d) 在起始亮度为100 cd/m²下器件工作寿命特性

Figure 5. (a) Normalized electroluminescence spectra of the devices with different NH₄SCN concentrations; (b) normalized electroluminescence spectra of the 0% NH₄SCN and (c) 20% NH₄SCN devices under different operating voltages, the inset shows a photograph of a working 20% NH₄SCN device; (d) operational life-time properties of the devices measured with an initial luminance of 100 cd/m².

DownLoad: Full-Size Img PowerPoint

表 1 不同NH₄SCN浓度钙钛矿薄膜的时间分辨光致发光的拟合参数总结

Table 1. Summarization of the fitting parameters for TRPL decay traces of the perovskite films with different NH₄SCN concentrations.

NH₄SCN concentration	$ A_1 $/%	$ {\rm{\tau}}_1 $/ns	$ A_2 $/%	$ {\rm{\tau}}_2 $/ns	${\rm{\tau} }_{\rm avg}$/ns
0%	93.47	0.87	6.53	10.10	1.47
10%	87.47	2.92	12.53	27.13	5.95
20%	92.97	4.93	7.03	42.06	7.54
40%	89.05	4.27	10.95	30.98	7.19

DownLoad: CSV

[1]	Sutherland B R, Sargent E H 2016 Nat. Photonics 10 295 Google Scholar
[2]	Kovalenko, M V, Protesescu L, Bodnarchuk, M I 2017 Science 358 745 Google Scholar
[3]	Van Le Q, Jang H W, Kim S Y 2018 Small Methods 2 1700419 Google Scholar
[4]	Kumawat N K, Liu X K, Kabra D, Gao F 2019 Nanoscale 11 2109 Google Scholar
[5]	段聪聪, 程露, 殷垚, 朱琳 2019 物理学报 68 158503 Google Scholar Duan C C, Cheng L, Yin Y, Zhu L 2019 Acta Phys. Sin. 68 158503 Google Scholar
[6]	吴海妍, 唐建新, 李艳青 2020 物理学报 69 138502 Google Scholar Wu H Y, Tang J X, Li Y Q 2020 Acta Phys. Sin. 69 138502 Google Scholar
[7]	Yuan F, Ran C, Zhang L, Dong H, Jiao B, Hou X, Li J, Wu Z 2020 ACS Energy Lett. 5 1062 Google Scholar
[8]	Xu W, Hu Q, Bai S, Bao C, Miao Y, Yuan Z, Borzda T, Barker A J, Tyukalova E, Hu Z, Kawecki M, Wang H, Yan Z, Liu X, Shi X, Uvdal K, Fahlman M, Zhang W, Duchamp M, Liu J M, Petrozza A, Wang J, Liu L M, Huang W, Gao F 2019 Nat. Photonics 13 418 Google Scholar
[9]	Chiba T, Hayashi Y, Ebe H, Hoshi K, Sato J, Sato S, Pu Y J, Ohisa S, Kido J 2018 Nat. Photonics 12 681 Google Scholar
[10]	Kim Y H, Kim S, Kakekhani A, Park J, Park J, Lee YH, Xu H, Nagane S, Wexler R B, Kim D H, Jo S H, Martínez-Sarti L, Tan P, Sadhanala A, Park GS, Kim Y W, Hu B, Bolink H J, Yoo S, Friend R H, Rappe A M, Lee T W 2021 Nat. Photonics 15 148 Google Scholar
[11]	Chu Z, Ye Q, Zhao Y, Ma F, Yin Z, Zhang X, You J 2021 Adv. Mater. 33 2007169 Google Scholar
[12]	Kumawat N K, Dey A, Kumar A, Gopinathan S P, Narasimhan K L, Kabra D 2015 ACS Appl. Mater. Interfaces 7 13119 Google Scholar
[13]	Ren Z, Yu J, Qin Z, Wang J, Sun J, Chan C C S, Ding S, Wang K, Chen R, Wong K S, Lu X, Yin W J, Choy W C H 2021 Adv. Mater. 33 2005570 Google Scholar
[14]	Dong Y, Wang Y K, Yuan F, Johnston A, Liu Y, Ma D, Choi M J, Chen B, Chekini M, Baek S W, Sagar L K, Fan J, Hou Y, Wu M, Lee S, Sun B, Hoogland S, Quintero-Bermudez R, Ebe H, Todorovic P, Dinic F, Li P, Kung H T, Saidaminov M I, Kumacheva E, Spiecker E, Liao L S, Voznyy O, Lu Z H, Sargent E H 2020 Nat. Nanotechnol. 15 668 Google Scholar
[15]	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
[16]	Gangishetty M K, Hou S, Quan Q, Congreve D N 2018 Adv. Mater. 30 1706226 Google Scholar
[17]	Vashishtha P, Ng M, Shivarudraiah S B, Halpert J E 2019 Chem. Mater. 31 83 Google Scholar
[18]	Cho H, Kim Y H, Wolf C, Lee H D, Lee T W 2018 Adv. Mater. 30 1704587 Google Scholar
[19]	Quan L N, Garcia de Arquer F P, Sabatini R P, Sargent E H 2018 Adv. Mater. 30 1801996 Google Scholar
[20]	Chen Z, Zhang C, Jiang X F, Liu M, Xia R, Shi T, Chen D, Xue Q, Zhao Y J, Su S, Yip H L, Cao Y 2017 Adv. Mater. 29 1603157 Google Scholar
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[22]	Wang Q, Ren J, Peng X F, Ji X X, Yang X H 2017 ACS Appl. Mater. Interfaces 9 29901 Google Scholar
[23]	Wang Z, Wang F, Sun W, Ni R, Hu S, Liu J, Zhang B, Alsaed A, Hayat T, Tan Z a 2018 Adv. Funct. Mater. 28 1804187 Google Scholar
[24]	Li Z, Chen Z, Yang Y, Xue Q, Yip H L, Cao Y 2019 Nat. Commun. 10 1027 Google Scholar
[25]	Wang Q, Wang X, Yang Z, Zhou N, Deng Y, Zhao J, Xiao X, Rudd P, Moran A, Yan Y, Huang J 2019 Nat. Commun. 10 5633 Google Scholar
[26]	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
[27]	Liu Y, Ono L K, Qi Y 2020 InfoMat 2 1095 Google Scholar
[28]	Wang D, Li W, Du Z, Li G, Sun W, Wu J, Lan Z 2020 ACS Appl. Mater. Interfaces 12 10579 Google Scholar
[29]	Liu Z, Liu D, Chen H, Ji L, Zheng H, Gu Y, Wang F, Chen Z, Li S 2019 Nanoscale Res. Lett. 14 304 Google Scholar
[30]	Fu W, Wang J, Zuo L, Gao K, Liu F, Ginger D S, Jen A K Y 2018 ACS Energy Lett. 3 2086 Google Scholar
[31]	Han S, Zhang H, Wang R, He Q 2021 Mat. Sci. Semicon. Proc. 127 105666 Google Scholar
[32]	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
[33]	Zhang X, Wu G, Yang S, Fu W, Zhang Z, Chen C, Liu W, Yan J, Yang W, Chen H 2017 Small 13 1700611 Google Scholar
[34]	Leung T L, Tam H W, Liu F, Lin J, Ng A M C, Chan W K, Chen W, He Z, Lončarić I, Grisanti L, Ma C, Wong K S, Lau Y S, Zhu F, Skoko Ž, Popović J, Djurišić A B 2019 Adv. Opt. Mater. 8 1901679 Google Scholar
[35]	Hu J, Oswald I W H, Stuard S J, Nahid M M, Zhou N, Williams O F, Guo Z, Yan L, Hu H, Chen Z, Xiao X, Lin Y, Yang Z, Huang J, Moran A M, Ade H, Neilson J R, You W 2019 Nat. Commun. 10 1276 Google Scholar
[36]	deQuilettes D W, Koch S, Burke S, Paranji R K, Shropshire A J, Ziffer M E, Ginger D S 2016 ACS Energy Lett. 1 438 Google Scholar
[37]	Pang P, Jin G, Liang C, Wang B, Xiang W, Zhang D, Xu J, Hong W, Xiao Z, Wang L, Xing G, Chen J, Ma D 2020 ACS Nano 14 11420 Google Scholar
[38]	Shen Y, Shen K C, Li Y Q, Guo M, Wang J, Ye Y, Xie F M, Ren H, Gao X, Song F, Tang J X 2020 Adv. Funct. Mater. 31 2006736 Google Scholar
[39]	Zhao X, Liu T, Kaplan A B, Yao C, Loo Y L 2020 Nano Lett. 20 8880 Google Scholar
[40]	Cai L, Liang D, Wang X, Zang J, Bai G, Hong Z, Zou Y, Song T, Sun B 2021 J. Phys. Chem. Lett. 12 1747 Google Scholar
[41]	Yu M, Yi C, Wang N, Zhang L, Zou R, Tong Y, Chen H, Cao Y, He Y, Wang Y, Xu M, Liu Y, Jin Y, Huang W, Wang J 2018 Adv. Opt. Mater. 7 1801575 Google Scholar
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[43]	Zou Y, Yuan Z, Bai S, Gao F, Sun B 2019 Mater. Today Nano 5 100028 Google Scholar
[44]	Liu X K, Xu W, Bai S, Jin Y, Wang J, Friend R H, Gao F 2021 Nat. Mater. 20 10 Google Scholar

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Vol. 70, Issue 19 - 2021-10-05

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