Mitigating interfacial carrier crowding by an ultrathin LiF interlayer towards efficient and stable perovskite light-emitting diodes

doi:10.1007/s44275-024-00018-9

Moore and More ›› 2025, Vol. 1 ›› Issue (3): 199-207.DOI: 10.1007/s44275-024-00018-9

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Mitigating interfacial carrier crowding by an ultrathin LiF interlayer towards efficient and stable perovskite light-emitting diodes

Xiaofei Zhang¹, Lin Wang¹, Lingmei Kong¹, Sheng Wang¹, Jun Dai³, Guohua Jia⁴, Xuyong Yang^1,2

1. Key Laboratory of Advanced Display and System Applications of Ministry of Education, Shanghai University, Shanghai, 200072, China;
2. Shanghai Engineering Research Center for Integrated Circuits and Advanced Display Materials, Shanghai University, Shanghai, 201899, China;
3. Department of Physics, Jiangsu University of Science and Technology, Zhenjiang, 212100, Jiangsu, China;
4. School of Molecular and Life Sciences, Curtin University, GPO Box U1987, Perth, WA, 6845, Australia

Received:2024-07-12 Revised:2024-10-04 Accepted:2024-10-23 Online:2025-11-29 Published:2024-12-26
Contact: Lin Wang,E-mail:lin_wang@shu.edu.cn;Xuyong Yang,E-mail:yangxy@shu.edu.cn
Supported by:
This work was supported by the financial support of the National Natural Science Foundation of China (62174104), the Shanghai Science and Technology Committee (22YF1413500), Program of Shanghai Academic/Technology Research Leader (22XD1421200), and Natural Science Foundation of Shanghai (23ZR1423300).

Mitigating interfacial carrier crowding by an ultrathin LiF interlayer towards efficient and stable perovskite light-emitting diodes

Xiaofei Zhang¹, Lin Wang¹, Lingmei Kong¹, Sheng Wang¹, Jun Dai³, Guohua Jia⁴, Xuyong Yang^1,2

1. Key Laboratory of Advanced Display and System Applications of Ministry of Education, Shanghai University, Shanghai, 200072, China;
2. Shanghai Engineering Research Center for Integrated Circuits and Advanced Display Materials, Shanghai University, Shanghai, 201899, China;
3. Department of Physics, Jiangsu University of Science and Technology, Zhenjiang, 212100, Jiangsu, China;
4. School of Molecular and Life Sciences, Curtin University, GPO Box U1987, Perth, WA, 6845, Australia

通讯作者: Lin Wang,E-mail:lin_wang@shu.edu.cn;Xuyong Yang,E-mail:yangxy@shu.edu.cn
作者简介:Xiaofei Zhang graduated from Hebei Normal University in 2020 with a bachelor’s degree. She obtained her master's degree from Jiangsu University of Science and Technology in 2023. She is currently a Ph.D. candidate supervised by Prof. Xuyong Yang. Her research focuses on perovskite light-emitting devices.
Lin Wang received her Ph.D. degree in nanomaterials and devices from Hubei University in 2018. After postdoctoral training in the group of Prof. Handong Sun in Nanyang Technological University, Singapore, she joined the Key Laboratory of Advanced Display and System Applications of Ministry of Education of Shanghai University as an assistant professor in 2020. Her research interests include the fabrication of semiconductor light-emitting nanomaterials and their optoelectronic devices.
Lingmei Kong received her master’s and Ph.D. degree from Shanghai University in 2021 and 2024, respectively. Her research work focuses on preparation of low dimensional semiconductor nanomaterials and their applications in light-emitting devices.
Sheng Wang received his Ph.D. degree from Jilin University. Then he joined the Key Laboratory of Advanced Display and System Applications of the Ministry of Education of Shanghai University as a postdoctoral fellow. He is now a lecturer at Shanghai University and his research interest is nanometer materials.
Jun Dai is the executive dean of the School of Science, Jiangsu University of Science and Technology. He obtained his Ph.D. degree from Southeast University in 2012. He then went to Nanyang Technological University as a visiting scholar in 2010–2011, and subsequently went to the University of WisconsinMadison as a visiting scholar in 2015–2016. His research interests include semiconductor optics.
Guohua Jia is an associate professor at Curtin University, Australia. He obtained his Ph.D. degree in chemistry in 2009 from City University of Hong Kong and subsequently worked as a postdoctoral fellow with Prof. Uri Banin at the Hebrew University of Jerusalem, Israel from 2010 to 2014. He commenced his current role as a group leader at Curtin University in 2015. His research interests focus on chemistry and physics of semiconductor nanocrystals, with particular emphasis on their properties and application in optoelectronic devices.
Xuyong Yang is a full professor at Shanghai University, China. He received his Ph.D. degree in microelectronics from Nanyang Technological University in Singapore in 2014, and worked as a postdoc at the same university prior to beginning his independent research career at Shanghai University. His research focuses primarily on design and fabrication of low dimensional semiconductor nanomaterials such as quantum dots and perovskite nanocrystals, as well as their applications in light-emitting devices.
基金资助:
This work was supported by the financial support of the National Natural Science Foundation of China (62174104), the Shanghai Science and Technology Committee (22YF1413500), Program of Shanghai Academic/Technology Research Leader (22XD1421200), and Natural Science Foundation of Shanghai (23ZR1423300).

Abstract

Abstract: Quasi-two-dimensional (quasi-2D) perovskite-based light-emitting diodes (PeLEDs) have attracted intensive attention due to their high quantum yields, tunable emission wavelengths, and solution-processing capability, showing great potential in next-generation display and lighting applications. However, further performance enhancement in PeLEDs is severely limited by the uncontrolled transfer of charge carriers under bias, leading to crowding of interfacial carriers and severe efficiency roll-off. Herein, we insert an ultra-thin dielectric buffer layer of lithium fluoride (LiF) into the electron transport layer (ETL) to regulate the transfer dynamics of electrons and passivate the interfacial defects simultaneously. The dielectric LiF interlayer can effectively reduce the efficiency roll-off in PeLEDs by improving the charge balance through preventing the overwhelming injection of electrons. Moreover, the fluoride anions from LiF can passivate the surface defects of the perovskite film, enhancing the radiative recombination. As a result, the LiF interlayer-assisted quasi-2D PeLED presents an outstanding external quantum efficiency (EQE) of 24.03% and a maximum brightness of 30 845 cd m^-2. The operational stability of the device is also extended, with a half-lifetime (T₅₀) of 71.28 min (at an initial luminance of 1 000 cd m^-2), which is 7.4-fold longer than that for the control device.

Key words: Perovskite light-emitting diodes, Efficiency roll-off, LiF interlayer, Charge balance, Defect passivation

摘要： Quasi-two-dimensional (quasi-2D) perovskite-based light-emitting diodes (PeLEDs) have attracted intensive attention due to their high quantum yields, tunable emission wavelengths, and solution-processing capability, showing great potential in next-generation display and lighting applications. However, further performance enhancement in PeLEDs is severely limited by the uncontrolled transfer of charge carriers under bias, leading to crowding of interfacial carriers and severe efficiency roll-off. Herein, we insert an ultra-thin dielectric buffer layer of lithium fluoride (LiF) into the electron transport layer (ETL) to regulate the transfer dynamics of electrons and passivate the interfacial defects simultaneously. The dielectric LiF interlayer can effectively reduce the efficiency roll-off in PeLEDs by improving the charge balance through preventing the overwhelming injection of electrons. Moreover, the fluoride anions from LiF can passivate the surface defects of the perovskite film, enhancing the radiative recombination. As a result, the LiF interlayer-assisted quasi-2D PeLED presents an outstanding external quantum efficiency (EQE) of 24.03% and a maximum brightness of 30 845 cd m^-2. The operational stability of the device is also extended, with a half-lifetime (T₅₀) of 71.28 min (at an initial luminance of 1 000 cd m^-2), which is 7.4-fold longer than that for the control device.

关键词: Perovskite light-emitting diodes, Efficiency roll-off, LiF interlayer, Charge balance, Defect passivation

Xiaofei Zhang, Lin Wang, Lingmei Kong, Sheng Wang, Jun Dai, Guohua Jia, Xuyong Yang. Mitigating interfacial carrier crowding by an ultrathin LiF interlayer towards efficient and stable perovskite light-emitting diodes[J]. Moore and More, 2025, 1(3): 199-207.

References

[1] Tan Z-K, Moghaddam RS, Lai ML, Docampo P, Higler R, Deschler F et al (2014) Bright light-emitting diodes based on organometal halide perovskite. Nat Nanotechnol 9:687-692. https://doi.org/10.1038/nnano.2014.149
[2] Fan M, Huang JP, Turyanska L, Bian ZF, Wang LC, Xu CY et al (2023) Efficient all-perovskite white light-emitting diodes made of in situ grown perovskite-mesoporous silica nanocomposites. Adv Funct Mater 23:2215032. https://doi.org/10.1002/adfm.202215032
[3] Chun FJ, Zhang BB, Gao YY, Wei XH, Zhang Q, Zheng WL et al (2024) Multicolour stretchable perovskite electroluminescent devices for user-interactive displays. Nat Photonics 18:856-863. https://doi.org/10.1038/s41566-024-01455-6
[4] Kong LM, Zhang XY, Li YG, Wang HR, Jiang YZ, Wang S et al (2021) Smoothing the energy transfer pathway in quasi-2D perovskite films using methanesulfonate leads to highly efficient light-emitting devices. Nat Commun 12:1246. https://doi.org/10.1038/s41467-021-21522-8
[5] Jiang YZ, Sun CJ, Xu J, Li SS, Cui MH, Fu XL et al (2022) Synthesis-on-substrate of quantum dot solids. Nature 612:679-684. https:// doi.org/https://doi.org/10.1038/s41586-022-05486-3
[6] An HJ, Baek SD, Kim DH, Myoung J-M (2022) Energy and charge dual transfer engineering for high-performance green perovskite light-emitting diodes. Adv Funct Mater 32:2112849. https://doi.org/10.1002/adfm.202112849
[7] Zhao XF, Tan Z-K (2019) Large-area near-infrared perovskite light-emitting diodes. Nat Photonics 14:215-218. https://doi.org/10.1038/s41566-019-0559-3
[8] Karlsson M, Yi ZY, Reichert S, Luo XY, Lin WH, Zhang ZY et al (2021) Mixed halide perovskites for spectrally stable and high-efficiency blue light-emitting diodes. Nat Commun 12:361. https://doi.org/10.1038/s41467-020-20582-6
[9] Kim Y-H, Park J, Kim S, Kim JS, Xu HX, Jeong S-H et al (2022) Exploiting the full advantages of colloidal perovskite nanocrystals for large-area efficient light-emitting diodes. Nat Nanotechnol 17:590-597. https://doi.org/10.1038/s41565-022-01113-4
[10] Li MM, Yang YG, Kuang ZY, Hao CJ, Wang SX, Lu FY et al (2024) Acceleration of radiative recombination for efficient perovskite LEDs. Nature 630:631-635. https://doi.org/10.1038/s41586-024-07460-7
[11] Nong YY, Yao JS, Li JQ, Xu LM, Yang Z, Li C et al (2024) Boosting external quantum efficiency of blue perovskite QLEDs exceeding 23% by trifluoroacetate passivation and mixed hole transportation design. Adv Mater 36:2402325. https://doi.org/10.1002/adma.202402325
[12] Jiang J, Chu ZM, Yin ZG, Li JZ, Yang YG, Chen JR et al (2022) Red perovskite light-emitting diodes with efficiency exceeding 25% realized by co-spacer cations. Adv Mater 34:2204460. https://doi.org/10.1002/adma.202204460
[13] Bai WH, Xuan TT, Zhao HY, Dong HR, Cheng XR, Wang L et al (2023) Perovskite light-emitting diodes with an external quantum efficiency exceeding 30%. Adv Mater 35:2302283. https://doi.org/10.1002/adma.202302283
[14] Sun CJ, Jiang YZ, Cui MH, Qiao L, Wei JL, Huang YM et al (2021) High-performance large-area quasi-2D perovskite light-emitting diodes. Nat Commun 12:2207. https://doi.org/10.1038/s41467-021-22529-x
[15] Han DY, Wang J, Agosta L, Zang Z, Zhao B, Kong LM et al (2023) Tautomeric mixture coordination enables efficient lead-free perovskite LEDs. Nature 622:7983. https://doi.org/10.1038/s41586-023-06514-6
[16] Diesing S, Zhang L, Zysman-Colman E, Samuel IDW (2024) A figure of merit for efficiency roll-off in TADF-based organic LEDs. Nature 627:747-753. https://doi.org/10.1038/s41586-024-07149-x
[17] Zhao LF, Astridge DD, Gunnarsson WB, Xu ZJ, Hong J, Scott J et al (2023) Thermal properties of polymer hole-transport layers influence the efficiency roll-off and stability of perovskite light-emitting diodes. Nano Lett 23:4785-4792. https://doi.org/10.1021/acs.nanolett.3c00148
[18] Ye YL, Wang JX, Qiu YL, Liu JH, Ye BQ, Yang ZX et al (2021) Ultra-low EQE roll-off and marvelous efficiency perovskite quantum-dots light-emitting-diodes achieved by ligand passivation. Nano Energy 90:106583. https://doi.org/10.1016/j.nanoen.2021.106583
[19] Cho H-H, Gorgon S, Hung H-C, Huang J-Y, Wu Y-R, Li F et al (2023) Efficient and bright organic radical light-emitting diodes with low efficiency roll-off. Adv Mater 35:2303666. https://doi.org/10.1002/adma.202303666
[20] Peng H, Xu YL, Zhou CJ, Pei RR, Miao JS, Liu H et al (2023) Donor extension on spiro-acridine enables highly efficient TADF-OLEDs with relieved efficiency roll-off. Adv Funct Mater 33:2211696. https://doi.org/10.1002/adfm.202211696
[21] Lin Y-K, Chen C-H, Wang Y-Y, Yu M-H, Yang J-W, Ni I-C et al (2023) Realizing high brightness quasi-2D perovskite light-emitting diodes with reduced efficiency roll-off via multifunctional interface engineering. Adv Sci 10:2302232. https://doi.org/10.1002/advs.202302232
[22] Goushi K, Yoshida K, Sato K, Adachi C (2012) Organic light-emitting diodes employing efficient reverse intersystem crossing for triplet-to-singlet state conversion. Nat Photonics 6:253-258. https://doi.org/10.1038/nphoton.2012.31.
[23] Zhang XF, Kong LM, Wang L, Chen T, Yang XY, Dai J (2023) A mixed organic-inorganic interlayer with tunable electrical properties enabling stable and efficient perovskite light-emitting diodes. IEEE Electron Device Lett 44:456-459. https://doi.org/10.1109/led.2023.3235764
[24] Wang Y, Teng Y, Lu P, Shen XY, Jia P, Lu M et al (2020) Low roll-off perovskite quantum dot lightemitting diodes achieved by augmenting hole mobility. Adv Funct Mater 30:1910140. https://doi.org/10.1002/adfm.201910140
[25] Li W, Li TX, Tong Y, Qi H, Zhang YQ, Guo YY et al (2023) Fabrication of highly luminescent quasi two-dimensional CsPbBr₃ perovskite films in high humidity air for light-emitting diodes. ACS Appl Mater Interfaces 15:36602-36610. https://doi.org/10.1021/acsami.3c07140
[26] An HJ, Baek SD, Kim DH, Myoung J-M (2022) Energy and charge dual transfer engineering for high performance green perovskite light-emitting diodes. Adv Funct Mater 32:2112849. https://doi.org/10.1002/adfm.202112849
[27] Guo ML, Lu Y, Cai XY, Shen Y, Qian XY, Ren H et al (2022) Interface engineering improves the performance of green perovskite light-emitting diodes. J Mater Chem C 10:2998-3005. https://doi.org/10.1039/d1tc05706e.
[28] Zhang TK, Long MZ, Pan LX, Ngai K, Qin MC, Xie FY et al (2020) Green perovskite light-emitting diodes with simultaneous high luminance and quantum efficiency through charge injection engineering. Sci Bull 65:1832-1839. https://doi.org/10.1016/j.scib.2020.06.024
[29] Kong LM, Zhang XY, Zhang CX, Wang L, Wang S, Cao F et al (2022) Stability of perovskite light-emitting diodes: existing issues and mitigation strategies related to both material and device aspects. Adv Mater 34:2205217. https://doi.org/10.1002/adma.202205217
[30] Salehi A, Ho S, Chen Y, Peng C, Yersin H, So F (2017) Highly efficient organic light-emitting diode using a low refractive index electron transport layer. Adv Opt Mater 5:1700197. https://doi.org/10.1002/adom.201700197
[31] Zou W, Li R, Zhang S, Liu Y, Wang N, Cao Y, et al (2018) Minimising efficiency roll-off in high-brightness perovskite light-emitting diodes. Nat Commun 9:608. https://doi.org/10.1038/s41467-018-03049-7
[32] Kong LM, Sun YQ, Zhao B, Ji KY, Feng J, Dong JC et al (2024) Fabrication of red-emitting perovskite LEDs by stabilizing their octahedral structure. Nature 631:73-79. https://doi.org/10.1038/s41586-024-07531-9
[33] Zhou W, Shen Y, Cao L-X, Lu Y, Tang Y-Y, Zhang K et al (2023) Manipulating ionic behavior with bifunctional additives for efficient sky-blue perovskite light-emitting diodes. Adv Funct Mater 33:2301425. https://doi.org/10.1002/adfm.202301425
[34] Zou C, Liu Y, Ginger DS, Lin LY (2020) Suppressing efficiency roll-off at high current densities for ultra-bright green perovskite light-emitting diodes. ACS Nano 14:5076-6086. https://doi.org/10.1021/acsnano.0c01817
[35] Yu MB, Mei XY, Qin TX, Zhuang RS, Hua Y, Zhang XL (2022) Modulating phase distribution and passivating surface defects of quasi-2D perovskites via potassium tetrafluoroborate for light-emitting diodes. Chem Eng J 450:138021. https://doi.org/10.1016/j.cej.2022.138021
[36] Ali MU, Miao JS, Cai JQ, Perepichka DF, Yang H, Meng H (2020) Boosting efficiency and curtailing the efficiency roll-off in green perovskite light-emitting diodes via incorporating ytterbium as cathode interface layer. ACS Appl Mater 12:18761-18768. https://doi.org/10.1021/acsami.0c00950
[37] Wang QG, Chen YJ, Yan C, Zeng XK, Fu XH, Pan LY et al (2023) Molecularly designing a passivation ETL to suppress EQE roll-off of PeLEDs. ACS Energy Lett 8:3710-3719. https://doi.org/10.1021/acsenergylett.3c01379
[38] Luo Y, Kong LM, Wang L, Shi XY, Yuan H, Li WQ et al (2022) A multifunctional ionic liquid additive enabling stable and efficient perovskite light-emitting diodes. Small 18:2200498. https://doi.org/10.1002/smll.202200498
[39] Li JH, Du PP, Guo QX, Sun L, Shen ZX, Zhu JX et al (2023) Efficient all-thermally evaporated perovskite light-emitting diodes for active-matrix displays. Nat Photonics 17:435-441. https://doi.org/10.1038/s41566-023-01177-1
[40] Zhuang LC, Zhai LL, Li YY, Ren H, Li MJ, Lau SP (2021) Mixed dimensional 0D/3D perovskite heterostructure for efficient green light-emitting diodes. J Mater Chem C 9:14318-14326. https://doi.org/10.1039/d1tc03611d
[41] Guo ZY, Zhang Y, Wang BZ, Wang LD, Zhou N, Qiu ZW et al (2021) Promoting energy transfer via manipulation of crystallization kinetics of quasi-2D perovskites for efficient green light-emitting diodes. Adv Mater 33:2102246. https://doi.org/10.1002/adma.202102246
[42] You MQ, Wang HR, Cao F, Zhang CX, Zhang T, Kong LM et al (2020) Improving efficiency and stability in quasi-2D perovskite light-emitting diodes by a multifunctional LiF interlayer. ACS Appl Mater Interfaces 12:43018-43023. https://doi.org/10.1021/acsami.0c11762
[43] Wang HR, Zhang XY, Wu QQ, Cao F, Yang DW, Shang YQ et al (2019) Trifluoroacetate induced small-grained CsPbBr₃ perovskite films result in efficient and stable light-emitting devices. Nat Commun 10:665. https://doi.org/10.1038/s41467-019-08425-5
[44] Kuang YH, Yang LP, Ma JM, Bie T, Zhang D, Xue YZ et al (2023) High-performance pure red quasi-two-dimensional perovskite light-emitting diodes with bifunctional potassium trifluoroacetate additive. ACS Materials Lett 11:2922-2928. https://doi.org/10.1021/acsmaterialslett.3c00557
[45] Zhang DZ, Fu YX, Zhan HM, Zhao CY, Gao X, Qin CJ et al (2022) Suppressing thermal quenching via defect passivation for efficient quasi-2D perovskite light-emitting diodes. Light Sci Appl 11:1-10. https://doi.org/10.1038/s41377-022-00761-4
[46] Guo ZY, Liang Y, Ni DY, Li L, Liu SC, Zhang Y et al (2023) Homogeneous phase distribution in Q-2D perovskites via co-assembly of spacer cations for efficient light-emitting diodes. Adv Mater 35:2302711. https://doi.org/10.1002/adma.202302711
[47] Li ZC, Chen ZM, Shi ZS, Zou GRX, Chu LH, Chen X-K et al (2023) Charge injection engineering at organic/inorganic heterointerfaces for high-efficiency and fast-response perovskite light-emitting diodes. Nat Commun 14:6441. https://doi.org/10.1038/s41467-023-41929-9
[48] Deng YY, Zhang ZG, Ren GH, Li ZQ, Liu CY, Guo WB (2023) An easily developed difunctional molecule enabling highly efficient and stable light-emitting diodes. Adv Funct Mater 33:2305423. https://doi.org/10.1002/adfm.202305423

Mitigating interfacial carrier crowding by an ultrathin LiF interlayer towards efficient and stable perovskite light-emitting diodes

Mitigating interfacial carrier crowding by an ultrathin LiF interlayer towards efficient and stable perovskite light-emitting diodes

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