发表机构
Gwangju Institute of Science and Technology (GIST); Max Planck Institute for the Structure and Dynamics of Matter; Universidad del País Vasco UPV/EHU; The Flatiron Institute（光州科学技术院; 马克斯·普朗克物质结构与动力学研究所; 巴斯克大学; 平顶山研究所）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
该研究针对三层1T'-WSe₂和1T'-WS₂，通过轨道选择性光激发调控层间距，结合模拟揭示了轨道-声子耦合诱导的层间距动力学，为调控层状材料电子性质提供了新途径。
AI 中文摘要
层间耦合控制着层状范德华过渡金属二硫族化合物的电子性质。我们研究了三层1T'-WSe₂和1T'-WS₂中，通过轨道选择性激发实现的光诱导层间距调控。实时含时密度泛函理论模拟表明，层间距的收缩或膨胀取决于硫族p轨道密度是从层间区域耗尽还是在层间区域积累。耦合晶格动力学的有效林德布拉德模型通过简化动力学重现了这些对比响应。单个有效激发态可捕获三层1T'-WSe₂中类余弦位移运动，而三层1T'-WS₂中平衡间距的偏移则需要两个具有不同电声耦合和弛豫通道的激发态。不同层间距下的静态计算表明，这些间距变化会改变电子带隙，并可进入不同的电子相。这些结果将轨道重新分布、载流子弛豫与层间呼吸运动关联起来，确立了轨道选择性光激发作为调控层状材料电子性质的一种途径。
英文摘要
Interlayer coupling controls the electronic properties of layered van der Waals transition metal dichalcogenides. We investigate light-induced control of the interlayer spacing through orbital-selective excitation in trilayer 1T'-WSe2 and 1T'-WS2. Real-time time-dependent density functional theory simulations show that the interlayer spacing contracts or expands depending on whether chalcogen p-orbital density is depleted from or accumulated in the interlayer region. Effective Lindblad models coupled to the lattice dynamics reproduce these contrasting responses with simplified dynamics. A single effective excited state captures the cosine-like displacive motion in trilayer 1T'-WSe2, whereas the shift of the equilibrium spacing in trilayer 1T'-WS2 requires two excited states with different electron-phonon couplings and relaxation channels. Static calculations at varied interlayer spacings indicate that these spacing changes modify the electronic gaps and could access different electronic phases. These results connect orbital redistribution, carrier relaxation, and interlayer breathing motion, and establish orbital-selective optical excitation as a route to tuning the electronic properties of layered materials.
Comments6figures
