Role of heterostacking of 2D lead chloride perovskites on photoluminescence
Role of heterostacking of 2D lead chloride perovskites on photoluminescence
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DOI：
10.1557/s43580-022-00358-4
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发表时间：
2022-11
期刊：
影响因子：
0.8
通讯作者：
D. R. Graupner;D. Kilin
中科院分区：
文献类型：
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作者：
D. R. Graupner;D. Kilin
二维有机-无机杂化的卤化铅钙钛矿由于其良好的可调性而在光伏和发光器件中引起了人们的兴趣。在这里，我们使用密度泛函理论来模拟不同厚度的二维卤化铅钙钛矿，并将其组合成垂直异质结构。用约化密度矩阵法处理的激发态动力学研究了钙钛矿模型的激发态光电性质。在常温下，基于分子动力学轨道上的On-the-Fly方法计算了非绝热耦合。利用基于密度矩阵的电子自由度运动方程计算了电子自由度的动力学。我们观察到，二维钙钛矿垂直堆积成异质结构时，光致发光强度比单独的二维钙钛矿增加了两个数量级。图形摘要
Two-dimensional organic–inorganic hybrid lead halide perovskites are of interest for photovoltaic and light-emitting devices due to their favorable properties that can be tuned. Here, we use density functional theory to model two-dimensional lead halide perovskites of different thicknesses and combined into vertical heterostructures. Excited-state dynamics treated by reduced density matrix method is used to examine the excited-state optoelectronic properties of the perovskite models. Nonadiabatic couplings were computed based on the on-the-fly approach along a molecular dynamics trajectory at ambient temperatures. The dynamics of electronic degrees of freedom were calculated using density matrix-based equation of motion for electronic degrees of freedom. We observe that the vertical stacking of two-dimensional perovskites into heterostructures shows an increase in photoluminescence intensity by two orders of magnitude when compared to the individual two-dimensional perovskites. Graphical abstract