Yang-hao Chan*, Mit H. Naik, Jonah B. Haber, Jeffrey B. Neaton, Steven G. Louie, Diana Y. Qiu* and Felipe H. da Jornada*,
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引用次数: 0
摘要
尽管范德瓦耳斯层间耦合很弱,但光诱导电荷垂直穿过原子薄界面的传输速度却快得惊人,可达 50 fs 以下。对电荷转移的早期理论理解是基于非相互作用的图景,忽略了主导此类材料光学特性的激子效应。我们采用了一种 ab initio 多体扰动理论方法,该方法明确考虑了异质结构中的激子和声子。我们的大规模第一性原理计算直接探究了激子-声子耦合在 WS2/MoS2 异质层电荷动力学中的作用。我们发现,在 300 K 时,MoS2 和 WS2 K 谷光激发激子的弛豫时间分别为 67 fs 和 15 fs,这为层内到层间的激子转移时间设定了下限,并与实验报告一致。我们进一步证明,电子-空穴关联促进了新的转移途径,否则非相互作用的电子和空穴是无法进入这些途径的。
Exciton–Phonon Coupling Induces a New Pathway for Ultrafast Intralayer-to-Interlayer Exciton Transition and Interlayer Charge Transfer in WS2–MoS2 Heterostructure: A First-Principles Study
Despite the weak, van der Waals interlayer coupling, photoinduced charge transfer vertically across atomically thin interfaces can occur within surprisingly fast, sub-50 fs time scales. An early theoretical understanding of charge transfer is based on a noninteracting picture, neglecting excitonic effects that dominate optical properties of such materials. We employ an ab initio many-body perturbation theory approach, which explicitly accounts for the excitons and phonons in the heterostructure. Our large-scale first-principles calculations directly probe the role of exciton–phonon coupling in the charge dynamics of the WS2/MoS2 heterobilayer. We find that the exciton–phonon interaction induced relaxation time of photoexcited excitons at the K valley of MoS2 and WS2 is 67 and 15 fs at 300 K, respectively, which sets a lower bound to the intralayer-to-interlayer exciton transfer time and is consistent with experiment reports. We further show that electron–hole correlations facilitate novel transfer pathways that are otherwise inaccessible to noninteracting electrons and holes.
期刊介绍:
Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including:
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