Dramatically Prolonged Photoexcited Carrier Lifetimes in Group-III Monochalcogenide Heterostructures through Stacking Modulation

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters Pub Date : 2025-04-23 DOI:10.1021/acs.jpclett.5c00700

Zixiao Yan, Yifan Wu, TianQi Bao, Yunxiao Ban, Lichuan Zhang, Yangyang Wan, Shi-Qi Li, Yuee Xie, Yuanping Chen, Xiaohong Yan

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Abstract

Modulating the carrier dynamics to achieve the effective separation of photoexcited carriers is crucial for enhancing photoelectric conversion efficiency and advancing high-performance optoelectronic devices. A prototype group-III monochalcogenide heterostructure, GaSe/GaTe, has been proposed to exhibit a superior light-harvesting capability and highly tunable charge separation characteristics via nonadiabatic molecular dynamics (NAMD) simulations. The significant influence of stacking patterns on carrier dynamics is revealed, with electron (hole) transfer occurring within 97 (40) to 390 (126) fs, while the carrier lifetime is dramatically prolonged from 12 to 213 ns, facilitating effective electron–hole (e-h) pair separation. Notably, the AA′ and A′A stacking configurations demonstrate remarkably extended carrier lifetimes of 213 and 161 ns, respectively, exceeding those observed in other 2D heterostructures. The weak nonadiabatic coupling and low-frequency phonon vibrational modes suppress e-h recombination, leading to a prolonged carrier lifetime. These findings offer atomic insights into stacking-dependent carrier dynamics, advancing 2D optoelectronic device design.

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通过堆叠调制大幅延长第 III 族单卤化物异质结构中的光激发载流子寿命

调制载流子动力学以实现光激载流子的有效分离是提高光电转换效率和推进高性能光电器件的关键。通过非绝热分子动力学（NAMD）模拟，提出了一种原型iii族单硫族异质结构GaSe/GaTe，该异质结构具有优越的光捕获能力和高度可调的电荷分离特性。电子（空穴）迁移发生在97 (40)~ 390 (126)fs之间，载流子寿命从12 ns大幅延长至213 ns，有利于电子-空穴（e-h）对的有效分离。值得注意的是，AA ‘和A ’ A堆叠构型的载流子寿命分别延长了213和161 ns，超过了其他二维异质结构。弱的非绝热耦合和低频声子振动模式抑制了e-h复合，导致载流子寿命延长。这些发现为堆积相关的载流子动力学提供了原子见解，推进了二维光电器件的设计。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

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.