Pressure-Driven Reverse Intersystem Crossing: New Path toward Bright Deep-Blue Emission of Lead-Free Halide Double Perovskites

Ma, Zhiwei1; Li, Qian2; Luo, Jiajun3,4; Li, Shunran3,4; Sui, Laizhi5; Zhao, Dianlong1; Yuan, Kaijun5; Xiao, Guanjun1; Tang, Jiang3,4; Quan, Zewei2; Zou, Bo1

2021-09-22

10.1021/jacs.1c06207

Journal of the American Chemical Society   影响因子和分区

0002-7863

1520-5126

Maximizing the regeneration of singlet excitons remains a considerable challenge in deep-blue emission systems to obtain low-cost, high-efficiency fluorescent materials. However, the formation of the long-lifetime triplet excitons generally dominates the radiative process, making it greatly difficult to harvest deep-blue emission with high color purity because of the depression of singlet excitons. Here, a very bright deep-blue emission in double perovskite Cs2Na0.4Ag0.6InCl6 alloyed with Bi doping (CNAICB) was successfully achieved by pressure-driven reverse intersystem crossing (RISC), an abnormal photophysical process of energy transfer from the excited triplet state back to the singlet. Therein, the inherently broad emission of CNAICB was associated with the self-trapped excitons (STEs) at excited triplet states, whereas the radiative recombination of STEs populated in excited singlet states was responsible for the observed deep-blue emission. Moreover, the deep-blue emission corresponds to Commission Internationale de L'Eclairage (CIE) coordinates (0.16, 0.06) at 5.01 GPa, which meets the requirement of Rec. 2020 display standards. Likewise, pressure was introduced as an efficient tool to rule out the possibility of the recombination of free excitons and clarify the long-standing conventional dispute over the origin of the low-wavelength emission of Cs2AgInCl6. Our study not only demonstrates that pressure can be a robust means to boost the deep-blue emission but also provides deep insights into the structure-property relationship of lead-free CNAICB double perovskites.

SCI ; EI

英语

NI论文

通讯

National Science Foundation of China[21725304,51761145048,22131006,12174144,11774125] ; National Key R&D Program of China[2019YFE0120300] ; Chinese Government[2017YFE0132300] ; Chemical Dynamics Research Center[21688102] ; China Postdoctoral Science Foundation[2021M690065] ; Australian Government[2017YFE0132300]

Chemistry

Chemistry, Multidisciplinary

WOS:000700883200030

AMER CHEMICAL SOC

Web of Science

1.Jilin Univ, Coll Phys, State Key Lab Superhard Mat, Changchun 130012, Jilin, Peoples R China
2.Southern Univ Sci & Technol SUSTech, Acad Adv Interdisciplinary Studies, Shenzhen Engn Res Ctr Frontier Mat Synth High Pre, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
3.Huazhong Univ Sci & Technol HUST, Sargent Joint Res Ctr, Wuhan Natl Lab Optoelect WNLO, Wuhan 430074, Peoples R China
4.Huazhong Univ Sci & Technol HUST, Sch Opt & Elect Informat, Wuhan 430074, Peoples R China
5.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China

Ma, Zhiwei,Li, Qian,Luo, Jiajun,et al. Pressure-Driven Reverse Intersystem Crossing: New Path toward Bright Deep-Blue Emission of Lead-Free Halide Double Perovskites[J]. Journal of the American Chemical Society,2021,143(37).

Ma, Zhiwei.,Li, Qian.,Luo, Jiajun.,Li, Shunran.,Sui, Laizhi.,...&Zou, Bo.(2021).Pressure-Driven Reverse Intersystem Crossing: New Path toward Bright Deep-Blue Emission of Lead-Free Halide Double Perovskites.Journal of the American Chemical Society,143(37).

Ma, Zhiwei,et al."Pressure-Driven Reverse Intersystem Crossing: New Path toward Bright Deep-Blue Emission of Lead-Free Halide Double Perovskites".Journal of the American Chemical Society 143.37(2021).