Citation: Tao Zhang, Simin Gong, Ping Chen, Qi Chen, Liwei Chen. Incorporation of a Polyfluorinated Acrylate Additive for High-Performance Quasi-2D Perovskite Light-Emitting Diodes[J]. Acta Physico-Chimica Sinica, ;2023, 39(12): 230102. doi: 10.3866/PKU.WHXB202301024 shu

Incorporation of a Polyfluorinated Acrylate Additive for High-Performance Quasi-2D Perovskite Light-Emitting Diodes

Tao Zhang ^{1, 2} ,
Simin Gong ³ ,
Ping Chen ^3,, ,
Qi Chen ^{1, 2,,} ,
Liwei Chen ^{2, 4,,}

1.
School of Nano-Tech and Nano-Bionics, University of Science and Technology of China, Hefei 230026, China
2.
i-Lab, CAS Key Laboratory of Nanophotonic Materials and Devices, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, Jiangsu Province, China
3.
Chongqing Key Laboratory of Micro & Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
4.
In-situ Center for Physical Sciences, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

Corresponding author: Ping Chen, pingchen@swu.edu.cn Qi Chen, qchen2011@sinano.ac.cn Liwei Chen, lwchen2018@sjtu.edu.cn
Received Date: 14 January 2023
Revised Date: 13 February 2023
Accepted Date: 14 February 2023
Available Online: 28 February 2023
Fund Project: the Ministry of Science and Technology of China 2021YFA1202802the National Natural Science Foundation of China 21875280the National Natural Science Foundation of China 21991150the National Natural Science Foundation of China 21991153the National Natural Science Foundation of China 22022205the CAS Project for Young Scientists in Basic Research YSBR-054the Special Foundation for Carbon Peak Neutralization Technology Innovation Program of Jiangsu Province BE2022026the Natural Science Foundation Project of Chongqing CSTB2022NSCQ-MSX0438

Quasi-two-dimensional (quasi-2D) perovskites are one of the most promising luminescent layer candidates for light-emitting diodes (LEDs) because of their excellent optoelectronic properties such as large exciton binding energy, efficient energy transfer, high photoluminescence quantum yield, and adjustable band gap. However, the formation of a large number of low-dimensional phases and surface/interface defects during solution processing of quasi-two-dimensional perovskite films gives rise to an increase in non-radiative recombination, resulting in deteriorated light-emitting diode performance. It is highly desirable to simultaneously realize low-dimensional phase formation inhibition and surface/interface defect passivation during quasi-two-dimensional perovskite film formation. Herein, we report a multifunctional additive, 1, 6-bis(acryloyloxy)-2, 2, 3, 3, 4, 4, 5, 5-octafluorohexane (OFHDODA), which has strong physical and chemical interactions with the PEA₂Cs₂Pb₃Br₁₀ precursor that can effectively suppress non-radiative recombination in the perovskite films. The distinct C＝C peak in the Fourier transform infrared spectroscopy (FTIR) spectra and the F 1s peak in the X-ray photoelectron spectroscopy (XPS) spectra showed that OFHDODA molecules were successfully incorporated into the perovskite films, and most OFHDODA molecules existed as monomers. With the addition of OFHDODA, the photoluminescence quantum yield (PLQY) of the perovskite film increased from 19.7% to 49.0%, and the PL emission wavelength red-shifted from 508 to 511 nm. It was demonstrated that hydrogen bond interactions between the polyfluorine structure and PEA⁺ can tune perovskite crystallization dynamics, which inhibit the formation of low-dimensional phases, as shown by the reduced peak intensities at 403 nm (n = 1), 434 nm (n = 2), and 465 nm (n = 3) in the absorption spectra. The strong Lewis base moiety of the ester groups passivates the unsaturated Pb²⁺ defects at the surface and grain boundaries of the perovskite films, as evidenced by the Pb 4f peak shift in the XPS spectra and the C＝O shift in the FTIR spectra. The trap-filled limiting voltage (V_TFL) decreased in both hole-only and electron-only devices, which also proves the reduction of Pb²⁺ defects. At the optimized OFHDODA concentration, the scanning electron microscopy (SEM) and atomic force microscopy (AFM) results from the perovskite films show lower roughness and smoother surface potential, which promotes superior interfacial contact. As a result, perovskite LEDs with a device structure of indium tin oxide glass/poly (9-vinylcarbazole)/perovskite/1, 3, 5-tris(1-phenyl-1H-benzimidazol-2-yl)benzene/8-hydroxyquinolinolato-lithium/Al exhibited an improved maximum external quantum efficiency (EQE) from 8.55% to 13.76%, improved maximum brightness from 16400 to 17620 cd∙m⁻², and increased lifetime from 8 min to 12 min. This process provides an effective way to suppress non-radiative recombination in quasi-2D perovskites via additive molecular structure design, leading to superior electroluminescence performance.
- Quasi-two-dimensional perovskite,
- Non-radiative recombination,
- Low-dimensional inhibition,
- Defect passivation,
- Polyfluorinated acrylate additive
1. [1]
  Yuan, M. J.; Quan, L. N.; Comin, R.; Walters, G.; Sabatini, R.; Voznyy, O.; Hoogland, S.; Zhao, Y. B.; Beauregard, E. M.; Kanjanaboos, P.; et al. Nat. Nanotechnol. 2016, 11 (10), 872. doi: 10.1038/nnano.2016.110 doi: 10.1038/nnano.2016.110
2. [2]
  Wang, N. N.; Cheng, L.; Ge, R.; Zhang, S. T.; Miao, Y. F.; Zou, W.; Yi, C.; Sun, Y.; Cao, Y.; Yang, R.; et al. Nat. Photonics 2016, 10 (11), 699. doi: 10.1038/nphoton.2016.185 doi: 10.1038/nphoton.2016.185
3. [3]
  Zhang, L.; Sun, C. J.; He, T. W.; Jiang, Y. Z.; Wei, J. L.; Huang, Y. M.; Yuan, M. J. Light. Sci. Appl. 2021, 10 (1), 61. doi: 10.1038/s41377-021-00501-0 doi: 10.1038/s41377-021-00501-0
4. [4]
  Liu, Y.; Cui, J. Y.; Du, K.; Tian, H.; He, Z. F.; Zhou, Q. H.; Yang, Z. L.; Deng, Y. Z.; Chen, D.; Zuo, X. B.; et al. Nat. Photonics 2019, 13 (11), 760. doi: 10.1038/s41566-019-0505-4 doi: 10.1038/s41566-019-0505-4
5. [5]
  Zou, G. R. X.; Chen, Z. M.; Li, Z. C.; Yip, H. L. Acta Phys. - Chim. Sin. 2021, 37 (4), 2009002. doi: 10.3866/PKU.WHXB202009002
6. [6]
  Karlsson, M.; Yi, Z. Y.; Reichert, S.; Luo, X. Y.; Lin, W. H.; Zhang, Z. Y.; Bao, C. X.; Zhang, R.; Bai, S.; Zheng, G. H. J.; et al. Nat. Commun. 2021, 12 (1), 361. doi: 10.1038/s41467-020-20582-6 doi: 10.1038/s41467-020-20582-6
7. [7]
  Guo, Z. Y.; Zhou, H. P. Acta Chim. Sin. 2021, 79 (3), 223. doi: 10.6023/a20100463
8. [8]
  Pang, P. Y.; Jin, G. R.; Liang, C.; Wang, B. Z.; Xiang, W.; Zhang, D. L.; Xu, J. W.; Hong, W.; Xiao, Z. W.; Wang, L.; et al. ACS Nano 2020, 14 (9), 11420. doi: 10.1021/acsnano.0c03765 doi: 10.1021/acsnano.0c03765
9. [9]
  Ban, M. Y.; Zou, Y. T.; Rivett, J. P. H.; Yang, Y. G.; Thomas, T. H.; Tan, Y. S.; Song, T.; Gao, X. Y.; Credgington, D.; Deschler, F.; et al. Nat. Commun. 2018, 9 (1), 3892. doi: 10.1038/s41467-018-06425-5 doi: 10.1038/s41467-018-06425-5
10. [10]
  Wang, C. H.; Han, D. B.; Wang, J. H.; Yang, Y. G.; Liu, X. Y.; Huang, S.; Zhang, X.; Chang, S.; Wu, K. F.; Zhong, H. Z. Nat. Commun. 2020, 11 (1), 6428. doi: 10.1038/s41467-020-20163-7 doi: 10.1038/s41467-020-20163-7
11. [11]
  Ma, D. X.; Lin, K. B.; Dong, Y. T.; Choubisa, H.; Proppe, A. H.; Wu, D.; Wang, Y. K.; Chen, B.; Li, P. C.; Fan, J. Z.; et al. Nature 2021, 599 (7886), 594. doi: 10.1038/s41586-021-03997-z doi: 10.1038/s41586-021-03997-z
12. [12]
  Fu, Y. X.; Zhang, D. Z.; Zhan, H. M.; Zhao, C. Y.; Cheng, Y. X.; Qin, C. J.; Wang, L. X. J. Phys. Chem. Lett. 2021, 12 (48), 11645. doi: 10.1021/acs.jpclett.1c03413 doi: 10.1021/acs.jpclett.1c03413
13. [13]
  Jiang, J.; Chu, Z. M.; Yin, Z. G.; Li, J. Z.; Yang, Y. G.; Chen, J. R.; Wu, J. L.; You, J. B.; Zhang, X. W. Adv. Mater. 2022, 34 (36), 2204460. doi: 10.1002/adma.202204460 doi: 10.1002/adma.202204460
14. [14]
  Xiang, T.; Li, T.; Wang, M. S.; Zhang, W.; Ahmadi, M.; Wu, X. Y.; Xu, T. F.; Xiao, M. Q.; Xu, L.; Chen, P. Nano Energy 2022, 95, 10700. doi: 10.1016/j.nanoen.2022.107000 doi: 10.1016/j.nanoen.2022.107000
15. [15]
  Yin, Y.; Guo, Z. D.; Chen, G. Y.; Zhang, H. F.; Yin, W. J. Acta Phys. -Chim. Sin. 2021, 37 (4), 2008048. doi: 10.3866/PKU.WHXB202008048
16. [16]
  Wang, R.; Xue, J. J.; Wang, K. L.; Wang, Z. K.; Luo, Y. Q.; David, F.; Xu, G. W.; Selbi, N.; Huang, T. Y.; Zhao, Y. P.; et al. Science 2019, 366, 1509. doi: 10.1126/science.aay9698 doi: 10.1126/science.aay9698
17. [17]
  Shi, Y. R.; Wang, K. L.; Lou, Y. H.; Zhang, D. B.; Chen, C. H.; Chen, J.; Ni, Y. X.; Öz, S.; Wang, Z. K.; Liao, L. S. Nano Energy 2022, 97, 17200. doi: 10.1016/j.nanoen.2022.107200 doi: 10.1016/j.nanoen.2022.107200
18. [18]
  Xu, L. M.; Li, J. H.; Cai, B.; Song, J. Z.; Zhang, F. J.; Fang, T.; Zeng, H. B. Nat. Commun. 2020, 11 (1), 3902. doi: 10.1038/s41467-020-17633-3 doi: 10.1038/s41467-020-17633-3
19. [19]
  Li, M. L.; Zhao, Y. P.; Qin, X. Q.; Ma, Q. S.; Lu, J. X.; Lin, K. B.; Xu, P.; Li, Y. Q.; Feng, W. J.; Zhang, W. H.; Wei, Z. H. Nano. Lett. 2022, 22 (6), 2490. doi: 10.1021/acs.nanolett.2c00276 doi: 10.1021/acs.nanolett.2c00276
20. [20]
  Shen, D. Y.; Ren, Z. W.; Li, Q. Y.; Luo, C. Z.; Xia, W. L.; Zheng, Z. S.; Ma, W. C.; Li, J.; Chen, Y. ACS Appl. Mater. Inter. 2022, 14 (18), 21636. doi: 10.1021/acsami.2c01859 doi: 10.1021/acsami.2c01859
21. [21]
  Jiang, X. Y.; Wang, F.; Wei, Q.; Li, H. S.; Shang, Y. Q.; Zhou, W. J.; Wang, C.; Cheng, P. H.; Chen, Q.; Chen, L. W.; et al. Nat. Commun. 2020, 11 (1), 1245. doi: 10.1038/s41467-020-15078-2 doi: 10.1038/s41467-020-15078-2
22. [22]
  Zhang, M. Y.; Chen, Q.; Xue, R. M.; Zhan, Y.; Wang, C.; Lai, J. Q.; Yang, J.; Lin, H. Z.; Yao, J. L.; Li, Y. W.; et al. Nat. Commun. 2019, 10 (1), 4593. doi: 10.1038/s41467-019-12613-8 doi: 10.1038/s41467-019-12613-8
23. [23]
  Lim, D. J.; Marks, N. A.; Rowles, M. R. Carbon 2020, 162, 475. doi: 10.1016/j.carbon.2020.02.064 doi: 10.1016/j.carbon.2020.02.064
24. [24]
  Tang, F.; Chen, Q.; Chen, L.; Ye, F. Y.; Cai, J. H.; Chen, L. W. Appl. Phys. Lett. 2016, 109 (12), 123301. doi: 10.1063/1.4963269 doi: 10.1063/1.4963269
25. [25]
  Chen, Q.; Chen, L.; Ye, F. Y.; Zhao, T.; Tang, F.; Rajagopal, A.; Jiang, Z.; Jiang, S. L.; Jen, A. K.; Xie, Y.; et al. Nano Lett. 2017, 17 (5), 3231. doi: 10.1021/acs.nanolett.7b00847 doi: 10.1021/acs.nanolett.7b00847
26. [26]
  Liu, J. C.; Tang, F.; Ye, F. Y.; Chen, Q.; Chen, L. W. Acta Phys. -Chim. Sin. 2017, 33 (10), 1934. doi: 10.3866/PKU.WHXB201715185
27. [27]
  Wang, C.; Zhang, C.; Li, R. F.; Chen, Q.; Qian, L.; Chen, L. W. Acta Phys. - Chim. Sin. 2022, 38 (8), 2104030. doi: 10.3866/PKU.WHXB202104030
1. [1]
  Xiaoyao YIN , Wenhao ZHU , Puyao SHI , Zongsheng LI , Yichao WANG , Nengmin ZHU , Yang WANG , Weihai SUN . Fabrication of all-inorganic CsPbBr₃ perovskite solar cells with SnCl₂ interface modification. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 469-479. doi: 10.11862/CJIC.20240309
2. [2]
  Fan JIA , Wenbao XU , Fangbin LIU , Haihua ZHANG , Hongbing FU . Synthesis and electroluminescence properties of Mn²⁺ doped quasi-two-dimensional perovskites (PEA)₂Pb_yMn_1-yBr₄. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1114-1122. doi: 10.11862/CJIC.20230473
3. [3]
  Binbin Liu , Yang Chen , Tianci Jia , Chen Chen , Zhanghao Wu , Yuhui Liu , Yuhang Zhai , Tianshu Ma , Changlei Wang . Hydroxyl-functionalized molecular engineering mitigates 2D phase barriers for efficient wide-bandgap and all-perovskite tandem solar cells. Acta Physico-Chimica Sinica, 2026, 42(1): 100128-0. doi: 10.1016/j.actphy.2025.100128
4. [4]
  Runhua Chen , Qiong Wu , Jingchen Luo , Xiaolong Zu , Shan Zhu , Yongfu Sun . Defective Ultrathin Two-Dimensional Materials for Photo-/Electrocatalytic CO₂ Reduction: Fundamentals and Perspectives. Acta Physico-Chimica Sinica, 2025, 41(3): 100019-0. doi: 10.3866/PKU.WHXB202308052
5. [5]
  Juntao Yan , Liang Wei . 2D S-Scheme Heterojunction Photocatalyst. Acta Physico-Chimica Sinica, 2024, 40(10): 2312024-0. doi: 10.3866/PKU.WHXB202312024
6. [6]
  Shouhao WAN , Yihang SHEN , Xiang GAO , Yang CHEN , Jiaqi LI , Cuie ZHAO . Two-dimensional MOFs/MXene composite for high-performance transparent zinc-ion hybrid supercapacitors. Chinese Journal of Inorganic Chemistry, 2026, 42(8): 1582-1592. doi: 10.11862/CJIC.20260077
7. [7]
  Lewang Yuan , Yaoyao Peng , Zong-Jie Guan , Yu Fang . Insights into the development of 2D covalent organic frameworks as photocatalysts in organic synthesis. Acta Physico-Chimica Sinica, 2025, 41(8): 100086-0. doi: 10.1016/j.actphy.2025.100086
8. [8]
  Limin Zhao , Kaiqiang Xu , Chuanbiao Bie . 2D COF photocatalyst with highly stabilized tautomeric transition and singlet oxygen generation. Acta Physico-Chimica Sinica, 2026, 42(4): 100216-0. doi: 10.1016/j.actphy.2025.100216
9. [9]
  Mengfei He , Chao Chen , Yue Tang , Si Meng , Zunfa Wang , Liyu Wang , Jiabao Xing , Xinyu Zhang , Jiahui Huang , Jiangbo Lu , Hongmei Jing , Xiangyu Liu , Hua Xu . Epitaxial Growth of Nonlayered 2D MnTe Nanosheets with Thickness-Tunable Conduction for p-Type Field Effect Transistor and Superior Contact Electrode. Acta Physico-Chimica Sinica, 2025, 41(2): 100016-0. doi: 10.3866/PKU.WHXB202310029
10. [10]
  Shantao Zhang , TianAo Hou , Yandong Wang , Zhimin Fang , Yu Wu , Haolin Wang , Tao Chen , Shuang Chen , Wenhua Zhang , Shengzhong (Frank) Liu , Shangfeng Yang . π-Conjugation-extended dinaphthocarbazole phosphonic acid as a hole-selective layer for inverted perovskite solar cells. Acta Physico-Chimica Sinica, 2026, 42(3): 100194-0. doi: 10.1016/j.actphy.2025.100194
11. [11]
  Ran HUO , Zhaohui ZHANG , Xi SU , Long CHEN . Research progress on multivariate two dimensional conjugated metal organic frameworks. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2063-2074. doi: 10.11862/CJIC.20240195
12. [12]
  Huanhuan XIE , Yingnan SONG , Lei LI . Two-dimensional single-layer BiOI nanosheets: Lattice thermal conductivity and phonon transport mechanism. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 702-708. doi: 10.11862/CJIC.20240281
13. [13]
  Haiyu Zhu , Zhuoqun Wen , Wen Xiong , Xingzhan Wei , Zhi Wang . 二维半金属/硅异质结中肖特基势垒高度的准确高效预测. Acta Physico-Chimica Sinica, 2025, 41(7): 100078-0. doi: 10.1016/j.actphy.2025.100078
14. [14]
  Chunling Qin , Shuang Chen , Hassanien Gomaa , Mohamed A. Shenashen , Sherif A. El-Safty , Qian Liu , Cuihua An , Xijun Liu , Qibo Deng , Ning Hu . Regulating HER and OER Performances of 2D Materials by the External Physical Fields. Acta Physico-Chimica Sinica, 2024, 40(9): 2307059-0. doi: 10.3866/PKU.WHXB202307059
15. [15]
  Renjie Xue , Chao Ma , Jing He , Xuechao Li , Yanning Tang , Lifeng Chi , Haiming Zhang . Catassembly in the Host-Guest Recognition of 2D Metastable Self-Assembled Networks. Acta Physico-Chimica Sinica, 2024, 40(9): 2309011-0. doi: 10.3866/PKU.WHXB202309011
16. [16]
  Shasha SUN , Weichun HUANG , Mengke WANG . Research progress of interface regulation strategies and applications of two‑dimensional MXenes. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1465-1482. doi: 10.11862/CJIC.20240430
17. [17]
  Jian Cao , Chang Liu , Danling Wang , Haichao Li , Lina Xu , Hongping Xiao , Shaoqi Zhan , Xiao He , Guoyong Fang . Machine learning potentials for property predictions of two-dimensional group-Ⅲ nitrides. Acta Physico-Chimica Sinica, 2026, 42(4): 100224-0. doi: 10.1016/j.actphy.2025.100224
18. [18]
  Lixing ZHANG , Yaowen WANG , Xu HAN , Junhong ZHOU , Jinghui WANG , Liping LI , Guangshe LI . Research progress in the synthesis of fluorine-containing perovskites and their derivatives. Chinese Journal of Inorganic Chemistry, 2025, 41(9): 1689-1701. doi: 10.11862/CJIC.20250007
19. [19]
  Lin He , Lin Chen , Rundong Chen , Xianlong Zhou , Shuai Zhang , Bingquan Xia . 二维Ta₂C助催化剂用于增强光催化H₂O₂合成及有机污染物降解. Acta Physico-Chimica Sinica, 2026, 42(11): 100367-. doi: 10.1016/j.actphy.2026.100367
20. [20]
  Yuhang Zhang , Weiwei Zhao , Hongwei Liu , Junpeng Lü . Progress on Self-Powered Photodetectors Based on Low-Dimensional Materials. Acta Physico-Chimica Sinica, 2025, 41(3): 100020-0. doi: 10.3866/PKU.WHXB202310004

Get Citation

PDF

XML

Metrics

PDF Downloads(11)
Abstract views(3976)
HTML views(344)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142