Doublet luminescence due to coexistence of excitons and electron-hole plasmas in optically excited CH3NH3PbBr3 single crystal

doi:10.1088/1674-1056/ac29b5

中国物理B ›› 2022, Vol. 31 ›› Issue (4): 47104-047104.doi: 10.1088/1674-1056/ac29b5

Doublet luminescence due to coexistence of excitons and electron-hole plasmas in optically excited CH₃NH₃PbBr₃ single crystal

Jie Wang(王杰)¹, Guang-Zhe Ma(马广哲)¹, Lu Cao(曹露)¹, Min Gao(高敏)², and Dong Shi(石东)^1,†

1 School of Optoelectronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, China;
2 School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 610054, China

收稿日期:2021-06-21 修回日期:2021-08-30 接受日期:2021-09-24 出版日期:2022-03-16 发布日期:2022-03-16
通讯作者: Dong Shi E-mail:dshi@uestc.edu.cn
基金资助:
Project supported by the National Natural Science Foundation of China (Grant No. 51872038).

Doublet luminescence due to coexistence of excitons and electron-hole plasmas in optically excited CH₃NH₃PbBr₃ single crystal

Jie Wang(王杰)¹, Guang-Zhe Ma(马广哲)¹, Lu Cao(曹露)¹, Min Gao(高敏)², and Dong Shi(石东)^1,†

1 School of Optoelectronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, China;
2 School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 610054, China

Received:2021-06-21 Revised:2021-08-30 Accepted:2021-09-24 Online:2022-03-16 Published:2022-03-16
Contact: Dong Shi E-mail:dshi@uestc.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Grant No. 51872038).

摘要/Abstract

摘要： Doublet luminescence from hybrid metal trihalide perovskite semiconductors is observed along with materials processing when high-quality single crystals are obtainable. Yet, the underlying physical mechanism remains poorly understood. Here, we report controllable solution-processed crystallization that affords high-quality CH₃NH₃PbBr₃ single crystals with atomically flat pristine surfaces. Front-face photoluminescence (PL) shows doublet luminescence components with variable relative intensities depending on the crystal surface conditions. We further find that the low-energy PL component with asymmetric spectral line-shape becomes predominant when the atomically flat crystal surfaces are passivated in the ion-abundant saturated solutions, while poor-quality single crystal with visually rough surface only gives the high-energy PL with symmetric line-shape. The asymmetric spectral line-shape of the low-energy PL matches perfectly with the simulated bandedge emission. Therefore, the low-energy PL component is attributable to the intrinsic bandedge emission from the crystal bulk while the high-energy one to surface-specific emission. Elliott fitting to the absorption data and multi-exponential fitting to the time-resolved photoluminescence traces jointly indicate the coexistence of excitons and electron-hole plasmas in optically excited CH₃NH₃PbBr₃ single crystals, thereby catching the physical merit that leads to the occurrence of doublet luminescence.

关键词: semiconductor, crystal, surface, luminescence

Abstract: Doublet luminescence from hybrid metal trihalide perovskite semiconductors is observed along with materials processing when high-quality single crystals are obtainable. Yet, the underlying physical mechanism remains poorly understood. Here, we report controllable solution-processed crystallization that affords high-quality CH₃NH₃PbBr₃ single crystals with atomically flat pristine surfaces. Front-face photoluminescence (PL) shows doublet luminescence components with variable relative intensities depending on the crystal surface conditions. We further find that the low-energy PL component with asymmetric spectral line-shape becomes predominant when the atomically flat crystal surfaces are passivated in the ion-abundant saturated solutions, while poor-quality single crystal with visually rough surface only gives the high-energy PL with symmetric line-shape. The asymmetric spectral line-shape of the low-energy PL matches perfectly with the simulated bandedge emission. Therefore, the low-energy PL component is attributable to the intrinsic bandedge emission from the crystal bulk while the high-energy one to surface-specific emission. Elliott fitting to the absorption data and multi-exponential fitting to the time-resolved photoluminescence traces jointly indicate the coexistence of excitons and electron-hole plasmas in optically excited CH₃NH₃PbBr₃ single crystals, thereby catching the physical merit that leads to the occurrence of doublet luminescence.

Key words: semiconductor, crystal, surface, luminescence

中图分类号: (Excited states and pairing interactions in model systems)

71.10.Li

71.20.Nr (Semiconductor compounds) 71.15.Qe (Excited states: methodology)

Jie Wang(王杰), Guang-Zhe Ma(马广哲), Lu Cao(曹露), Min Gao(高敏), and Dong Shi(石东). Doublet luminescence due to coexistence of excitons and electron-hole plasmas in optically excited CH₃NH₃PbBr₃ single crystal[J]. 中国物理B, 2022, 31(4): 47104-047104.

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Doublet luminescence due to coexistence of excitons and electron-hole plasmas in optically excited CH₃NH₃PbBr₃ single crystal

Doublet luminescence due to coexistence of excitons and electron-hole plasmas in optically excited CH₃NH₃PbBr₃ single crystal

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