Temperature-Dependent Recombination Dynamics of Photocarriers in CsPbBr3 Microcrystals Revealed by Ultrafast Terahertz Spectroscopy

IF 8 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Advanced Optical Materials Pub Date : 2024-09-17 DOI:10.1002/adom.202401162

Sheng H. Lee, Kyeongdeuk Moon, Muhammad Shoaib, Charles N. B. Pedorella, Kellen O'Brien, Meng-Ju Sher, Seokhyoung Kim, Tyler L. Cocker

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Abstract

The ultrafast dynamics of photoexcited charge carriers are studied in micron-scale crystals composed of the inorganic perovskite CsPbBr₃ with time-resolved terahertz spectroscopy. Exciting with photon energy close to the band edge, it is found that a fast (<10 ps) decay emerges in the terahertz photoconductivity with increasing pump fluence and decreasing temperature, dominating the dynamics at 4 K. The fluence-dependent dynamics can be globally fit by a nonlinear recombination model, which reveals that the influence of different nonlinear recombination mechanisms in the studied pump fluence range depends on temperature. Whereas the Auger scattering rate decreases with decreasing temperature from 77 to 4 K, the radiative recombination rate increases by three orders of magnitude. Spectroscopically, the terahertz photoconductivity resembles a Drude response at all delays, yet an additional Lorentz component due to an above-bandwidth resonance is needed to fully reproduce the data.

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超快太赫兹光谱揭示 CsPbBr3 微晶中光电载流子的温度依赖性重组动力学

利用时间分辨太赫兹光谱法研究了由无机包晶 CsPbBr3 组成的微米级晶体中光激发电荷载流子的超快动力学。研究发现，随着泵浦通量的增加和温度的降低，太赫兹光电导率会出现快速（10 ps）衰减，在 4 K 时，这种动态占主导地位。从 77 到 4 K，奥杰散射率随着温度的降低而降低，而辐射重组率则增加了三个数量级。从光谱学角度看，太赫兹光电导在所有延迟下都类似于德鲁德响应，但要完全再现数据，还需要额外的洛伦兹分量，这是由于带宽以上的共振造成的。

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来源期刊

Advanced Optical Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-OPTICS

CiteScore

13.70

自引率

6.70%

发文量

883

审稿时长

1.5 months

期刊介绍： Advanced Optical Materials, part of the esteemed Advanced portfolio, is a unique materials science journal concentrating on all facets of light-matter interactions. For over a decade, it has been the preferred optical materials journal for significant discoveries in photonics, plasmonics, metamaterials, and more. The Advanced portfolio from Wiley is a collection of globally respected, high-impact journals that disseminate the best science from established and emerging researchers, aiding them in fulfilling their mission and amplifying the reach of their scientific discoveries.