了解MoSSe双层中与扭转角相关的载流子寿命

IF 4.6 2区 化学 Q2 CHEMISTRY, PHYSICAL
Tianqi Bao, Ning Li, Xue Jiang, Jijun Zhao and Yan Su*, 
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引用次数: 0

摘要

具有可调谐层间相互作用的二维(2D)材料在光电和光催化应用方面具有巨大的潜力。了解载流子动力学对双子星层扭转角的依赖是必要的,因为它直接影响器件效率。本研究采用时间依赖密度泛函理论(TD-DFT)和非绝热分子动力学(NAMD)研究了具有ii型带取向的Janus MoSSe双层中与扭转角相关的载流子动力学。模拟表明,超快电荷转移时间约为70和500秒,很大程度上与多个中间态的扭转角无关。相反,电子-空穴复合时间在很大程度上依赖于扭转角,在扭转构型(21.8°和38.2°)中延长至133 ns,而在高对称双层结构(0.0°和60.0°)中延长至57 ns。扭曲双层结构的随机性削弱了层间相互作用,减少了非绝热耦合和相干时间,从而延长了载流子寿命。这些发现为设计用于高效光伏和长寿命光催化剂的二维材料提供了有价值的指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Understanding Twist-Angle-Dependent Carrier Lifetimes in MoSSe Bilayer

Understanding Twist-Angle-Dependent Carrier Lifetimes in MoSSe Bilayer

Two-dimensional (2D) materials with tunable interlayer interactions hold immense potential for optoelectronic and photocatalytic applications. Understanding the dependence of carrier dynamics on twist angle in Janus bilayers is essential, as it directly impacts device efficiency. This study employs time-dependent density functional theory (TD-DFT) and nonadiabatic molecular dynamics (NAMD) to investigate twist-angle-dependent carrier dynamics in Janus MoSSe bilayers with type-II band alignment. Simulations reveal ultrafast charge transfer times of approximately 70 and 500 fs, largely independent of the twist angle due to multiple intermediate states. In contrast, the electron–hole recombination times depend strongly on twist angles, extending up to 133 ns for twisted configurations (21.8° and 38.2°) compared to 57 ns in high-symmetry bilayers (0.0° and 60.0°). Structural randomness in twisted bilayers weakens interlayer interactions, reducing nonadiabatic coupling and coherence time, which collectively prolong carrier lifetimes. These findings offer valuable guidance for designing 2D materials for high-efficiency photovoltaics and long-durable photocatalysts.

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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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