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中国物理学会期刊

二维Re6Se8Cl2中反常层依赖的光生载流子寿命

Anomalous layer-dependence of photogenerated carrier lifetime in two-dimensionalRe6Se8Cl2

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  • 基于量子限域效应的层数调控是调控二维(2D)光电器件性能的常用策略。通常,增加层数会减小二维材料的带隙,因而缩短光生载流子的寿命。本文通过第一性原理计算结合非绝热分子动力学(NAMD)模拟研究二维材料Re6Se8Cl2中光生载流子寿命反常的层数依赖行为。具体而言,Re6Se8Cl2的光生载流子寿命随层数的增加先增大后减小,双层体系表现出最长的载流子寿命。这种反常的行为来源于带隙和电子-声子(e-ph)耦合的共同作用。尽管Re6Se8Cl2的带隙随层数的增加呈指数衰减,加速了载流子复合,但内外层Re-Cl键的电荷重新分布抑制了高频声子模并削弱了e-ph耦合,进而抑制光生载流子复合。这些发现加深了对二维材料层数和光生载流子寿命间关系的理解,并为设计高性能光电器件提供了理论基础。

     

    Regulating the number of layers in two-dimensional (2D) materials is a well-known strategy for enhancing the performance of optoelectronic devices. Unfortunately, as the layer number increases, the lifetime of photogenerated carriers often shortens due to narrowing band gap, limiting the optimization of device performance. Polarization in 2D materials, known to inhibit carrier recombination, offers a potential solution to this limitation. Incorporating electrostatic potential difference into layer number regulation may reveal new insights into controlling the photogenerated carrier lifetimes. Recently, the superatomic crystal represented by Re6Se8Cl2 has attracted attention for inducing electrostatic potential difference through asymmetric Cl termination, presenting new opportunities for designing high-performance optoelectronic devices. In this study, we reveal an anomalous layer-dependent behavior of photogenerated carrier lifetime. Specifically, the carrier lifetime increases initially and then decreases as the number of layers increases. This anomaly behavior stems from combined effects: while the band gap of Re6Se8Cl2 decreases exponentially with additional layers, accelerating recombination, electrostatic potential difference driven charge redistribution weakens electron-phonon coupling, suppressing recombination. Our findings suggest that electrostatic potential difference in few-layer materials like Re6Se8Cl2 enhances optoelectronic properties by extending carrier lifetime and improving light absorption.

     

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