1. Time-Domain Ab Initio Insights into the Reduced Nonradiative Electron–Hole Recombination in ReSe2/MoS2 van der Waals Heterostructure
- Author
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Tianzhao Li, Biyu Song, Jinge Wu, Miao Zhou, Wenzhen Dou, Xiamin Hao, Qingling Meng, Yizhen Jia, Weijuan Hu, and Shuwei Zhai
- Subjects
Materials science ,Band gap ,Ab initio ,Heterojunction ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Molecular physics ,0104 chemical sciences ,Vibronic coupling ,Molecular dynamics ,symbols.namesake ,symbols ,General Materials Science ,Density functional theory ,Charge carrier ,Physical and Theoretical Chemistry ,van der Waals force ,0210 nano-technology - Abstract
Two-dimensional (2D) ReSe2 has attracted considerable interest due to its unique anisotropic mechanical, optical, and exitonic characteristics. Recent transient absorption experiments demonstrated a prolonged lifetime of photoexcited charge carriers by stacking ReSe2 with MoS2, but the underlying mechanism remains elusive. Here, by combining time-domain density functional theory with nonadiabatic molecular dynamics, we investigate the electronic properties and charge carrier dynamics of 2D ReSe2/MoS2 van der Waals (vdW) heterostructure. ReSe2/MoS2 has a type II band alignment that exhibits spatially distinguished conduction and valence band edges, and a built-in electric field is formed due to interface charge transfer. Remarkably, in spite of the decreased band gap and increased decoherence time, we demonstrate that the photocarrier lifetime of ReSe2/MoS2 is ∼5 times longer than that of ReSe2, which originates from the greatly reduced nonadiabatic coupling that suppresses electron-hole recombination, perfectly explaining the experimental results. These findings not only provide physical insights into experiments but also shed light on future design and fabrication of functional optoelectronic devices based on 2D vdW heterostructures.
- Published
- 2021
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