Wrinkles are a unique class of surface corrugations present over diverse length scales from Kinneyia-type wrinkles in Archean-era sedimentary fossils to nanoscopic crinkling in two-dimensional crystals. Lately, the role of wrinkles on graphene has been subject to debate as devices based on graphene progress towards commercialization. While the topology and electronic structure of graphene wrinkles is known, data on wrinkle geometrical effects on molecular adsorption patterns and resonance states is lacking. Here, we report molecular superstructures and enhancement of free-molecular electronic states of pentacene on graphene wrinkles. A new trend is observed where the pentacene energy gap scales with wrinkle height, as wrinkles taller than 2 nm significantly screen metal induced hybridization. Combined with density functional theory calculations, the impact of wrinkles in tuning molecular growth modes and electronic structure is clarified at room-temperature. These results suggest the need to rethink wrinkle engineering in modular devices based on graphene and related 2D materials interfacing with electronically active molecules.

皱纹是一类独特的表面皱纹，存在于不同的长度范围内，从太古时代沉积化石中的Kinneyia型皱纹到二维晶体的纳米皱纹。近来，皱纹在石墨烯上的作用一直受到争议，因为基于石墨烯的装置正朝着商业化的方向发展。尽管已知石墨烯皱纹的拓扑结构和电子结构，但缺乏有关皱纹几何效应对分子吸附模式和共振态的数据。在这里，我们报告分子并列结构和石墨烯皱纹上并五苯的自由分子电子态的增强。观察到一种新趋势，其中并五苯能隙随着皱纹高度而缩放，因为高于2 nm的皱纹会显着屏蔽金属诱导的杂交。结合密度泛函理论计算，在室温下，皱纹对调节分子生长模式和电子结构的影响是明确的。这些结果表明，需要重新考虑基于石墨烯和与电子活性分子连接的相关2D材料的模块化设备中的皱纹工程。