Composition engineering to obtain efficient hybrid perovskite light-emitting diodes

Abstract

Metal halide perovskites have received considerable attention in the field of electroluminescence, and the external quantum efficiency of perovskite light-emitting diodes has exceeded 20%. CH₃NH₃PbBr₃ has been intensely investigated as an emitting layer in perovskite light-emitting diodes. However, perovskite films comprising CH₃NH₃PbBr₃ often exhibit low surface coverage and poor crystallinity, leading to high current leakage, severe nonradiative recombination, and limited device performance. Herein, we demonstrate a rationale for composition engineering to obtain high-quality perovskite films. We first reduce pinholes by adding excess CH₃NH₃Br to the actual CH₃NH₃PbBr₃ films, and we then add CsBr to improve the crystalline quality and to passivate nonradiative defects. As a result, the (CH₃NH₃)_1−xCs_xPbBr₃ based perovskite light-emitting diodes exhibit significantly improved external quantum and power efficiencies of 6.97% and 25.18 lm/W, respectively, representing an improvement in performance dozens of times greater than that of pristine CH₃NH₃PbBr₃-based perovskite light-emitting diodes. Our study demonstrates that composition engineering is an effective strategy for enhancing the device performance of perovskite light-emitting diodes.

Graphical abstract

Keywords

perovskite / light-emitting diode (LED) / composition engineering / ion doping

References

[1] 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. Bright light-emitting diodes based on organometal halide perovskite. Nature Nanotechnology, 2014, 9(9): 687–692

[2] Song J, Li J, Li X, Xu L, Dong Y, Zeng H. Quantum dot light-emitting diodes based on inorganic perovskite cesium lead halides (CsPbX₃). Advanced Materials, 2015, 27(44): 7162–7167

[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. Perovskite energy funnels for efficient light-emitting diodes. Nature Nanotechnology, 2016, 11(10): 872–877

[4] 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. Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes. Science, 2015, 350(6265): 1222–1225

[5] Wei Z, Perumal A, Su R, Sushant S, Xing J, Zhang Q, Tan S T, Demir H V, Xiong Q. Solution-processed highly bright and durable cesium lead halide perovskite light-emitting diodes. Nanoscale, 2016, 8(42): 18021–18026

[6] Wei Z, Xing J. The rise of perovskite light-emitting diodes. Journal of Physical Chemistry Letters, 2019, 10(11): 3035–3042

[7] Wang J, Wang N, Jin Y, Si J, Tan Z K, Du H, Cheng L, Dai X, Bai S, He H, Ye Z, Lai M L, Friend R H, Huang W. Interfacial control toward efficient and low-voltage perovskite light-emitting diodes. Advanced Materials, 2015, 27(14): 2311–2316

[8] Li G, Rivarola F W R, Davis N J L K, Bai S, Jellicoe T C, de la Peña F, Hou S, Ducati C, Gao F, Friend R H, Greenham N C, Tan Z K. Highly efficient perovskite nanocrystal light-emitting diodes enabled by a universal crosslinking method. Advanced Materials, 2016, 28(18): 3528–3534

[9] Wang N, Cheng L, Ge R, Zhang S, Miao Y, Zou W, Yi C, Sun Y, Cao Y, Yang R, Wei Y, Guo Q, Ke Y, Yu M, Jin Y, Liu Y, Ding Q, Di D, Yang L, Xing G, Tian H, Jin C, Gao F, Friend R H, Wang J, Huang W. Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells. Nature Photonics, 2016, 10(11): 699–704

[10] Xiao Z, Kerner R A, Zhao L, Tran N L, Lee K M, Koh T W, Scholes G D, Rand B P. Efficient perovskite light-emitting diodes featuring nanometre-sized crystallites. Nature Photonics, 2017, 11(2): 108–115

[11] Zhang L, Yang X, Jiang Q, Wang P, Yin Z, Zhang X, Tan H, Yang Y M, Wei M, Sutherland B R, Sargent E H, You J. Ultra-bright and highly efficient inorganic based perovskite light-emitting diodes. Nature Communications, 2017, 8(1): 15640

[12] Wu Y, Wei C, Li X, Li Y, Qiu S, Shen W, Cai B, Sun Z, Yang D, Deng Z, Zeng H. In situ passivation of PbBr₆^4– octahedra toward blue luminescent CsPbBr₃ nanoplatelets with near 100% absolute quantum yield. ACS Energy Letters, 2018, 3(9): 2030–2037

[13] Xing J, Zhao Y, Askerka M, Quan L N, Gong X, Zhao W, Zhao J, Tan H, Long G, Gao L, Yang Z, Voznyy O, Tang J, Lu Z H, Xiong Q, Sargent E H. Color-stable highly luminescent sky-blue perovskite light-emitting diodes. Nature Communications, 2018, 9(1): 3541

[14] Lu J, Feng W, Mei G, Sun J, Yan C, Zhang D, Lin K, Wu D, Wang K, Wei Z. Ultrathin PEDOT:PSS enables colorful and efficient perovskite light-emitting diodes. Advanced Science, 2020, 7(11): 2000689

[15] Lin K, Xing J, Quan L N, de Arquer F P G, Gong X, Lu J, Xie L, Zhao W, Zhang D, Yan C, Li W, Liu X, Lu Y, Kirman J, Sargent E H, Xiong Q, Wei Z. Perovskite light-emitting diodes with external quantum efficiency exceeding 20 percent. Nature, 2018, 562(7726): 245–248

[16] Chiba T, Hayashi Y, Ebe H, Hoshi K, Sato J, Sato S, Pu Y J, Ohisa S, Kido J. Anion-exchange red perovskite quantum dots with ammonium iodine salts for highly efficient light-emitting devices. Nature Photonics, 2018, 12(11): 681–687

[17] Zhao X, Tan Z K. Large-area near-infrared perovskite light-emitting diodes. Nature Photonics, 2020, 14(4): 215–218

[18] Cao Y, Wang N, Tian H, Guo J, Wei Y, Chen H, Miao Y, Zou W, Pan K, He Y, Cao H, Ke Y, Xu M, Wang Y, Yang M, Du K, Fu Z, Kong D, Dai D, Jin Y, Li G, Li H, Peng Q, Wang J, Huang W. Perovskite light-emitting diodes based on spontaneously formed submicrometre-scale structures. Nature, 2018, 562(7726): 249–253

[19] 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. Rational molecular passivation for high-performance perovskite light-emitting diodes. Nature Photonics, 2019, 13(6): 418–424

[20] Meredith P, Armin A. LED technology breaks performance barrier. Nature, 2018, 562(7726): 197–198

[21] Service R F. Perovskite LEDs begin to shine. Science, 2019, 364(6444): 918

[22] Quan L N, García de Arquer F P, Sabatini R P, Sargent E H. Perovskites for light emission. Advanced Materials, 2018, 30(45): 1801996

[23] Xie L, Song P, Shen L, Lu J, Liu K, Lin K, Feng W, Tian C, Wei Z. Revealing the compositional effect on the intrinsic long-term stability of perovskite solar cells. Journal of Materials Chemistry A, 2020, 8(16): 7653–7658

[24] Kanwat A, Choi W C, Seth S, Jang J. Doping and photon induced defect healing of hybrid perovskite thin films: an approach towards efficient light emitting diodes. ChemNanoMat: Chemistry of Nanomaterials for Energy, Biology and More, 2019, 5(5): 666–673

[25] Xu Z, Liu Z, Li N, Tang G, Zheng G, Zhu C, Chen Y, Wang L, Huang Y, Li L, Zhou N, Hong J, Chen Q, Zhou H. A thermodynamically favored crystal orientation in mixed formamidinium/methylammonium perovskite for efficient solar cells. Advanced Materials, 2019, 31(24): 1900390

[26] Si J, Liu Y, Wang N, Xu M, Li J, He H, Wang J, Jin Y. Green light-emitting diodes based on hybrid perovskite films with mixed cesium and methylammonium cations. Nano Research, 2017, 10(4): 1329–1335

[27] Yang X, Chu Z, Meng J, Yin Z, Zhang X, Deng J, You J. Effects of organic cations on the structure and performance of quasi-two-dimensional perovskite based light-emitting diodes. Journal of Physical Chemistry Letters, 2019, 10(11): 2892–2897

[28] Prakasam V, Di Giacomo F, Abbel R, Tordera D, Sessolo M, Gelinck G, Bolink H J. Efficient perovskite light-emitting diodes: Effect of composition, morphology, and transport layers. ACS Applied Materials & Interfaces, 2018, 10(48): 41586–41591

[29] Naphade R, Zhao B, Richter J M, Booker E, Krishnamurthy S, Friend R H, Sadhanala A, Ogale S. High quality hybrid perovskite semiconductor thin films with remarkably enhanced luminescence and defect suppression via quaternary alkyl ammonium salt based treatment. Advanced Materials Interfaces, 2017, 4(19): 1700562

[30] Prasanna R, Gold-Parker A, Leijtens T, Conings B, Babayigit A, Boyen H G, Toney M F, McGehee M D. Band gap tuning via lattice contraction and octahedral tilting in perovskite materials for photovoltaics. Journal of the American Chemical Society, 2017, 139(32): 11117–11124

[31] Xie L, Lin K, Lu J, Feng W, Song P, Yan C, Liu K, Shen L, Tian C, Wei Z. Efficient and stable low-bandgap perovskite solar cells enabled by a CsPbBr₃-cluster assisted bottom-up crystallization approach. Journal of the American Chemical Society, 2019, 141(51): 20537–20546

[32] Min H, Kim M, Lee S U, Kim H, Kim G, Choi K, Lee J H, Seok S I. Efficient, stable solar cells by using inherent bandgap of a-phase formamidinium lead iodide. Science, 2019, 366(6466): 749–753

Acknowledgements

The work was financially supported by the National Natural Science Foundation of China (Grant Nos. 51802102, 21805101, and 51902110), Natural Science Foundation of Fujian Province (No. 2019J01057), Promotion Program for Young and Middle-aged Teacher in Science and Technology Research of Huaqiao University (No. ZQN-PY607), and Scientific Research Funds of Huaqiao University (Nos. 16BS201, 17BS409, and 19BS105).

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