Journal
NANOSCALE
Volume 9, Issue 35, Pages 13245-13256Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7nr03951d
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Funding
- U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- EPSRC [EP/K013564/1]
- Extreme Science and Engineering Discovery Environment (XSEDE)
- NSF [TG-DMR120049, TG-DMR150017]
- Queen's Fellow Award through the startup grant [M8407MPH]
- EPSRC
- Arizona State University startup funds
- EPSRC [EP/K013459/1, EP/P022561/1, EP/K013564/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/P022561/1, 1612621, EP/K013564/1, EP/K013459/1] Funding Source: researchfish
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Hybrid van der Waals (vdW) heterostructures composed of two-dimensional (2D) layered materials and self-assembled organic molecules are promising systems for electronic and optoelectronic applications with enhanced properties and performance. Control of molecular assembly is therefore paramount to fundamentally understand the nucleation, ordering, alignment, and electronic interaction of organic molecules with 2D materials. Here, we report the formation and detailed study of highly ordered, crystalline monolayers of C-60 molecules self-assembled on the surface of WSe2 in well-ordered arrays with large grain sizes (similar to 5 mu m). Using high-resolution scanning tunneling microscopy (STM), we observe a periodic 2 x 2 superstructure in the C-60 monolayer and identify four distinct molecular appearances. Using vdW-corrected ab initio density functional theory (DFT) simulations, we determine that the interplay between vdW and Coulomb interactions as well as adsorbate-adsorbate and adsorbate-substrate interactions results in specific rotational arrangements of the molecules forming the superstructure. The orbital ordering through the relative positions of bonds in adjacent molecules creates a charge redistribution that links the molecule units in a long-range network. This rotational superstructure extends throughout the self-assembled monolayer and opens a pathway towards engineering aligned hybrid organic/inorganic vdW heterostructures with 2D layered materials in a precise and controlled way.
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