Exciton recombination mechanisms in solution grown single crystalline CsPbBr3 perovskite

Exciton recombination mechanisms in solution grown single crystalline CsPbBr3 perovskite
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溶液生长单晶 CsPbBr3 钙钛矿中的激子复合机制

DOI:
10.1016/j.jlumin.2020.117471
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发表时间:
2020-10
影响因子:
3.6
通讯作者:
Cao Dawei
Cao Dawei
中科院分区:
物理与天体物理2区
文献类型:
--
作者:
Yuan Youwen;Chen Mingming;Yang Shuaiheng;Shen Xuemin;Liu Yuan;Cao Dawei

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卤化铅钙钛矿由于在光伏技术和发光器件领域取得了巨大成功,近年来引起了人们的极大关注。在本工作中,得益于我们最近在溶液中生长高质量CsPbBr3单晶的工作,我们详细地研究了全无机钙钛矿型CsPbBr3的激子光致发光(PL)性质在87℃-297℃范围内的依赖温度的发光和拉曼光谱。从随温度变化的光致发光强度中提取激子结合能为37±22.7 meV。此外,与普通半导体相比,发光峰值能量表现出复杂的行为。随着温度的升高,发光光谱在223K以下蓝移,而在223K-293K范围内红移。理论研究表明,CsPbBr3在223K以下的能带演化主要由热膨胀控制,而在更高的温度下,电子-声子相互作用的贡献占主导地位。同时,发光光谱的展宽主要归因于激子-纵向光学声子散射。我们的结果可能有助于更好地理解未来全无机钙钛矿型CsPbBr3基发光器件的发光行为。
Lead halide perovskites have attracted tremendous attention recently due to their great success in the fields of photovoltaic technologies and light-emitting devices. In this work, the excitonic photoluminescence (PL) properties of all-inorganic perovskite CsPbBr3were investigated in detailviatemperature-dependent PL and Raman spectroscopy in the range of 87 K–297 K, benefiting from our recent work on solution growth of high-quality CsPbBr3single crystals. The exciton binding energy was extracted as 37 ± 2.7 meV from temperature-dependent PL emission intensity. Furthermore, the PL emission peak energy showed complicated behaviors compared to common semiconductors. With the increase of temperature, the PL emission spectrum blueshifted below 223 K, while it was redshifted in the range of 223 K–293 K. Theoretical research indicated that the thermal expansion governs the energy bandgap evolution of CsPbBr3below 223 K, while for higher temperatures, the contribution of electron-phonon interaction became dominant. Meanwhile, the broadening of the PL emission spectrum was mainly attributed to the exciton-longitudinal optical phonon scattering. Our results may contribute to a better understanding of the luminescence behaviors in all-inorganic perovskite CsPbBr3-based light-emitting devices in the future.
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