Transformation between the Dark and Bright Self-Trapped Excitons in Lead-Free Double-Perovskite Cs2NaBiCl6 under Pressure

Jiang, Jutao1,2; Niu, Guangming1,3; Sui, Laizhi1; Wang, Xiaowei1; Zhang, Yutong1; Li Che3; Wu, Guorong1; Yuan, Kaijun1,2; Yang, Xueming1,4

2021-08-05

10.1021/acs.jpclett.1c02072

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

Understanding the relationships between the structure and the properties in lead-free double perovskites is significant for their applications in the optoelectronic field. Here the nonluminous Cs2NaBiCl6 crystal exhibits an unexpected broadband dual-color emission as the external pressure is increased to 6.77 GPa. The emission intensity is remarkably enhanced with further compression to 8.50 GPa. By analyzing the results of in situ high-pressure experiments and the density functional theory, we conclude that the dual-color emission is attributed to singlet self-trapped excitons (STEs) and triplet STEs, respectively. This phenomenon originates from the tilting and twisting of [BiCl6](3-) caused by the transition of cubic Cs2NaBiCl6 to the tetragonal phase. Notably, the transformation between the dark and bright STEs in the Cs2NaBiCl6 crystal is demonstrated by ultrafast transient absorption experiments under different pressures. This work not only offers deep insight into the structure-property relationship in lead-free double perovskites but also opens the door for the design of new lead-free double perovskites.

SCI ; EI

英语

NI论文

其他

Chemical Dynamics Research Center[21688102] ; National Natural Science Foundation of China (NSFC)[21873099,21922306] ; Key Technology Team of the Chinese Academy of Sciences[GJJSTD20190002] ; Liaoning Revitalization Talents Program[XLYC1907154]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000683816500029

AMER CHEMICAL SOC

20213310780950

Chlorine compounds ; Crystals ; Density functional theory ; Excitons ; Perovskite ; Sodium compounds

Minerals:482.2 ; Probability Theory:922.1 ; Crystalline Solids:933.1

Web of Science

1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Dalian Maritime Univ, Sch Sci, Dept Phys, Dalian 116026, Peoples R China
4.Southern Univ Sci & Technol, Coll Sci, Dept Chem, Shenzhen 518055, Peoples R China

Jiang, Jutao,Niu, Guangming,Sui, Laizhi,et al. Transformation between the Dark and Bright Self-Trapped Excitons in Lead-Free Double-Perovskite Cs2NaBiCl6 under Pressure[J]. Journal of Physical Chemistry Letters,2021,12(30):7285-7292.

Jiang, Jutao.,Niu, Guangming.,Sui, Laizhi.,Wang, Xiaowei.,Zhang, Yutong.,...&Yang, Xueming.(2021).Transformation between the Dark and Bright Self-Trapped Excitons in Lead-Free Double-Perovskite Cs2NaBiCl6 under Pressure.Journal of Physical Chemistry Letters,12(30),7285-7292.

Jiang, Jutao,et al."Transformation between the Dark and Bright Self-Trapped Excitons in Lead-Free Double-Perovskite Cs2NaBiCl6 under Pressure".Journal of Physical Chemistry Letters 12.30(2021):7285-7292.