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Pressure-induced robust emission in a zero-dimensional hybrid metal halide (C9NH20)6Pb3Br12
Matter and Radiation at Extremes ( IF 5.1 ) Pub Date : 2021-08-25 , DOI: 10.1063/5.0058821
Mengting Chen 1 , Songhao Guo 1 , Kejun Bu 1 , Sujin Lee 2 , Hui Luo 1 , Yiming Wang 1 , Bingyan Liu 1 , Zhipeng Yan 1 , Hongliang Dong 1 , Wenge Yang 1 , Biwu Ma 2 , Xujie Lü 1
Affiliation  

Zero-dimensional (0D) hybrid metal halides are under intensive investigation owing to their unique physical properties, such as the broadband emission from highly localized excitons that is promising for white-emitting lighting. However, fundamental understanding of emission variations and structure–property relationships is still limited. Here, by using pressure processing, we obtain robust exciton emission in 0D (C9NH20)6Pb3Br12 at room temperature that can survive to 80 GPa, the recorded highest value among all the hybrid metal halides. In situ experimental characterization and first-principles calculations reveal that the pressure-induced emission is mainly caused by the largely suppressed phonon-assisted nonradiative pathway. Lattice compression leads to phonon hardening, which considerably weakens the exciton–phonon interaction and thus enhances the emission. The robust emission is attributed to the unique structure of separated spring-like [Pb3Br12]6− trimers, which leads to the outstanding stability of the optically active inorganic units. Our findings not only reveal abnormally robust emission in a 0D metal halide, but also provide new insight into the design and optimization of local structures of trimers and oligomers in low-dimensional hybrid materials.

中文翻译:

零维混合金属卤化物 (C9NH20)6Pb3Br12 中的压力诱导稳健发射

零维 (0D) 混合金属卤化物由于其独特的物理特性而受到深入研究,例如高度局域激子的宽带发射,有望用于发白光。然而,对排放变化和结构-性质关系的基本理解仍然有限。在这里,通过使用压力处理,我们在室温下在 0D (C 9 NH 20 ) 6 Pb 3 Br 12中获得了稳定的激子发射,可以承受 80 GPa,这是所有混合金属卤化物中记录的最高值。就地实验表征和第一性原理计算表明,压力诱导发射主要是由很大程度上受抑制的声子辅助非辐射途径引起的。晶格压缩导致声子硬化,这大大削弱了激子 - 声子相互作用,从而增强了发射。强大的发射归因于分离的弹簧状 [Pb 3 Br 12 ] 6-三聚体的独特结构,这导致光学活性无机单元具有出色的稳定性。我们的研究结果不仅揭示了 0D 金属卤化物中异常稳健的发射,而且还为低维混合材料中三聚体和低聚物的局部结构的设计和优化提供了新的见解。
更新日期:2021-09-23
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