AI 中文总结
通过角分辨光电子能谱结合Holstein模型模拟,揭示C₆₀薄膜电子结构随层数的非单调演化,确立层数为调控分子薄膜电子结构与多体相互作用的有效参数。
AI 中文摘要
晶态C₆₀是一种分子固体,其电子性质源于分子间跳跃、电子关联及电子-振动耦合的相互作用。与通常通过扭转角调控相互作用强度的莫尔范德华异质结构不同,分子材料提供了互补的调控途径,其中层数、分子取向和衬底配准是实验可实现的控制参数。本文报道了对C₆₀薄膜从单层到体相极限的系统性厚度依赖角分辨光电子能谱研究。源自最高占据分子轨道(HOMO)的能带呈现非单调演化:中等厚度薄膜表现出更大的带宽、更小的有效质量,以及明显的类能隙和子带特征。实验趋势结合霍斯坦(Holstein)模型模拟表明,中等厚度 regime 下分子间有效电子耦合增强,电子-声子诱导的谱重正化也随之增强。这些结果明确了C₆₀薄膜中的维度交叉,并确立层数作为调控分子薄膜电子结构和多体相互作用的有效旋钮。
英文摘要
Crystalline C$_{60}$ is a molecular solid whose electronic properties emerge from the interplay of intermolecular hopping, electron correlations, and electron-vibration coupling. Unlike moir$\rm\acute{e}$ van der Waals heterostructures, where interaction strength is commonly tuned by twist angle, molecular materials offer a complementary route in which layer number, molecular orientation, and substrate registry provide experimentally accessible control parameters. Here we present a systematic thickness-dependent angle-resolved photoemission study of C$_{60}$ films, spanning the monolayer to the bulk limit. The HOMO-derived band exhibits a non-monotonic evolution: the intermediate-thickness film shows larger bandwidth, reduced effective mass, and pronounced gap-like and sub-band features. The experimental trends, together with Holstein-model simulations, point to strengthened effective intermolecular electronic coupling and enhanced electron-phonon-induced spectral renormalization in the intermediate-thickness regime. These results identify a dimensional crossover in C$_{60}$ films and establish layer number as an effective knob for engineering electronic structure and many-body interactions in molecular thin films.
Comments10 pages, 4 figures; accepted for publication in Nano Letters