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堆叠极性控制MoSe2/MoS2异质结构中的层间光载流子动力学

Stacking Polarity-Controlled Interlayer Photocarrier Dynamics in MoSe2/MoS2 Heterostructures

Gbenga S. Agunbiade, Ting Zheng, Hui Zhao

arXiv 2607.25963首次发表:更新:

AI 中文总结

研究MoSe2/MoS2异质结构中层间光载流子动力学,通过比较2H和3R双层MoS2及设计3R堆叠界面终端,用超快泵浦-探测光谱法解析电荷转移动力学,实现层间激子寿命调谐,揭示堆叠极性对光载流子动力学的控制作用。

AI 中文摘要

控制层间光载流子动力学对于范德华异质结构的光电应用至关重要,但确定性和空间均匀的调谐策略仍然有限。本文表明堆叠极性为MoSe2/MoS2异质结构中的光载流子动力学提供了一个全局控制参数。通过比较六方(2H)和菱方(3R)MoS2双层,并在3R堆叠中设计相反的界面终端,我们使用超快泵浦-探测光谱法解析了依赖堆叠的层间电荷转移动力学。2H异质结构中的电荷转移比实验分辨率快,而3R异质结构显示出可时间分辨的电荷转移,其速度根据堆叠极性从0.25减慢到0.37 ps。此外,层间激子寿命从约40 ps调谐到约170 ps。这些效应源于3R MoS2中堆叠诱导的层极化,它调制了界面波函数重叠。

英文摘要

Control of interlayer photocarrier dynamics is central to optoelectronic applications of van der Waals heterostructures, yet deterministic and spatially uniform tuning strategies remain limited. Here we show that stacking polarity provides a global control parameter for photocarrier dynamics in MoSe$_2$/MoS$_2$ heterostructures. By comparing hexagonal (2H) and rhombohedral (3R) MoS$_2$ bilayers and engineering opposite interface terminations in 3R stacking, we resolve stacking-dependent interlayer charge-transfer dynamics using ultrafast pump--probe spectroscopy. While charge transfer in the 2H heterostructure occurs faster than the experimental resolution, the 3R heterostructures show time-resolvable charge transfer that slows from $0.25$ to $0.37$~ps depending on stacking polarity. Furthermore, the interlayer exciton lifetime is tuned from $\sim$$40$ to $\sim$$170$~ps. These effects arise from stacking-induced layer polarization in 3R MoS$_2$, which modulates interfacial wavefunction overlap.

Journal refNano Letters 26, 7564 (2026)

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