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Microscopic morphology independence in linear absorption cross-section of CsPbBr 3 nanocrystals
Science China Materials ( IF 6.8 ) Pub Date : 2021-01-13 , DOI: 10.1007/s40843-020-1555-1
Fengying Zhang , Yuchen Liu , Shiqian Wei , Junsheng Chen , Ying Zhou , Rongxing He , Tõnu Pullerits , Kaibo Zheng

Multiple morphologies of colloidal perovskite nanocrystals (NCs) diversify their optical and electronic properties. Among them, the linear absorption cross-section (σ) is a primary parameter to determine their intrinsic photophysical features, and consequently, application potential. Herein, three morphologies of all-inorganic hybrid colloidal perovskite CsPbBr3 NCs, nanocubes (NBs), nanoplatelets (NLs), and nanowires (NWs), were targeted, and their linear σ values were obtained through femtosecond transient absorption (TA) spectroscopy analysis. At high excitation energy well above the bandgap, the σ per particle of all CsPbBr3 NCs linearly increased with the particle volume (VNC) regardless of the morphology with the value of σ400 = 9.45 × 104 cm−1 × VNC (cm2). Density functional theory (DFT) calculation confirmed the negligible influence of shapes on the optical selection rules. The Einstein spontaneous emission coefficients calculated from the σ values define the intrinsic radiative recombination rate. However, reduced size dependence is observed when the excitation energy is close to the bandgap (i.e., at 460 nm) with the value of σ460 = 2.82 × 108 cm0.65 × (VNC)0.45 (cm2). This should be ascribed to the discrete energy levels as well as lower density of states close to the band edge for perovskite NCs. These results provide in-depth insight into the optical characteristics for perovskite NCs.



中文翻译:

CsPbBr 3纳米晶体的线性吸收截面中的微观形态独立性

胶态钙钛矿纳米晶体(NCs)的多种形态使其光学和电子特性多样化。其中,线性吸收截面(σ)是确定其固有的光物理特征以及因此具有应用潜力的主要参数。本文以全无机杂化胶体钙钛矿CsPbBr 3 NCs,纳米立方(NBs),纳米血小板(NLs)和纳米线(NWs)的三种形态为目标,并通过飞秒瞬态吸收(TA)光谱分析获得了它们的线性σ值。 。在远高于带隙的高激发能下,所有CsPbBr 3 NC的每个粒子的σ随粒子体积线性增加(V NC)不管与值形态的σ 400 = 9.45×10 4厘米-1 × V NC(厘米2)。密度泛函理论(DFT)的计算证实了形状对光学选择规则的影响可忽略不计。根据σ值计算出的爱因斯坦自发发射系数定义了固有辐射复合率。然而,减小的尺寸依赖性,观察到当激励能量是接近带隙(即,在460nm)同值σ 460 = 2.82×10 8厘米0.65 ×(V NC0.45(厘米2)。这应归因于钙钛矿型NC的离散能级以及靠近带边缘的较低态密度。这些结果为钙钛矿NC的光学特性提供了深入的了解。

更新日期:2021-01-18
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