Nonequilibrium Charge-Density-Wave Melting in 1T-TaS2 Triggered by Electronic Excitation: A Real-Time Time-Dependent Density Functional Theory Study,The Journal of Physical Chemistry Letters

当前位置： X-MOL 学术 › J. Phys. Chem. Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Nonequilibrium Charge-Density-Wave Melting in 1T-TaS2 Triggered by Electronic Excitation: A Real-Time Time-Dependent Density Functional Theory Study
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2022-06-17 , DOI: 10.1021/acs.jpclett.2c01352
Juhyung Lee ₁ , Junhyeok Bang _{2,

3} , Joongoo Kang ₁

Affiliation

Ultrafast charge transfer in van der Waals (vdW) heterostructures enables efficient control of two-dimensional material properties through strong optical absorption and subsequent carrier transfer. Here, using real-time time-dependent density functional theory coupled to molecular dynamics, we investigated the nonequilibrium dynamics of charge-density-wave (CDW) melting in 1T-TaS₂ triggered by ultrafast charge transfer in 1T-TaS₂/MoSe₂ or WSe₂ heterostructures. Despite the fast and sufficient charge transfer from the MoSe₂ (or WSe₂) “electrode” to the 1T-TaS₂ layer, the electronic excitation of the vdW heterostructure does not lead to the nonthermal CDW transition of 1T-TaS₂. Instead, the TaS₂ lattice is heated by carrier–lattice scattering, leading to thermal CDW melting at high ionic temperatures. The lack of nonthermal melting follows from the fact that the time scale of carrier recombination in 1T-TaS₂ is similar to or faster than that of charge transfer. These findings provide physical insights into understanding the CDW melting dynamics in vdW heterostructures under nonequilibrium conditions.

中文翻译：

电子激发触发的 1T-TaS2 中的非平衡电荷密度波熔化：实时时间相关密度泛函理论研究

范德华 (vdW) 异质结构中的超快电荷转移能够通过强光吸收和随后的载流子转移来有效控制二维材料特性。在这里，我们使用与分子动力学耦合的实时时间相关密度泛函理论，研究了由 1 T -TaS 2 中的超快电荷转移触发的 1 T -TaS 2 中的电荷密度波 ( CDW )_熔化的非平衡_动力学/ MoSe ₂或WSe ₂异质结构。_{尽管从 MoSe 2}（或 WSe ₂）“电极”到 1 T -TaS ₂的电荷转移速度快且足够层，vdW异质结构的电子激发不会导致1 T -TaS ₂的非热CDW转变。相反，TaS ₂晶格被载流子-晶格散射加热，导致热 CDW 在高离子温度下熔化。非热熔化的缺乏源于这样一个事实，即 1 T -TaS ₂中载流子复合的时间尺度与电荷转移的时间尺度相似或更快。这些发现为理解非平衡条件下 vdW 异质结构中的 CDW 熔化动力学提供了物理见解。

更新日期：2022-06-17

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11