论文标题

计算无机钙钛矿纳米晶体中的Biexciton转移

Calculation of the biexciton shift in nanocrystals of inorganic perovskites

论文作者

Nguyen, T. P. T., Blundell, S. A., Guet, C.

论文摘要

我们计算了无机perovskites cspbbr3和cspBi3的纳米晶体(NCS)的TRION和BIEXCITON(相对于单个激子)的发射频率的变化。计算使用包络功能K.P模型与自洽的Hartree-fock结合使用,并以多体扰动理论的最低(第二)顺序(第二)顺序(第二)顺序对载波相关能量进行处理。在发射之前,假定TRION和BIEXCITON中的载体在带缘之前的基态放宽。发现CSPBBR3和CSPBI3的理论转移与可用的实验数据相吻合,其中包括低温单点测量值,尽管可能在1.5阶的系统上很小,这可以证明这可以证明,这可以证明这可以通过略微高估的定位常量和更高的第三级和更高级别的序列来解释。考虑到这一水平的一致性,我们估计CSPBBR3的地面Biexciton偏移是NC的10-20 MEV订单的红移,其边缘长度为12 nm。该值中间是CSPBBR3 NC的众多高温测量值,从大的红移100 MEV到几个MEV的蓝光变化。

We calculate the shift in emission frequency of the trion and biexciton (relative to that of the single exciton) for nanocrystals (NCs) of inorganic perovskites CsPbBr3 and CsPbI3. The calculations use an envelope-function k.p model combined with self-consistent Hartree-Fock and a treatment of the intercarrier correlation energy in the lowest (second) order of many-body perturbation theory. The carriers in the trion and biexciton are assumed to have relaxed nonradiatively to the ground state at the band edge before emission occurs. The theoretical trion shifts for both CsPbBr3 and CsPbI3 are found to be in fair agreement with available experimental data, which include low-temperature single-dot measurements, though are perhaps systematically small by a factor of order 1.5, which can plausibly be explained by a combination of a slightly overestimated dielectric constant and omitted third- and higher-order terms in the correlation energy. Taking this level of agreement into account, we estimate that the ground-state biexciton shift for CsPbBr3 is a redshift of order 10-20 meV for NCs with an edge-length of 12 nm. This value is intermediate among the numerous high-temperature measurements on NCs of CsPbBr3, which vary from large redshifts of order 100 meV to blueshifts of several meV.

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