Structural transitions at the bilayer graphene-methanol interface from ab initio molecular dynamics.

Area of Science:

• Materials Science
• Computational Chemistry
• Surface Science

Background:

• Tailoring atomic structures in 2D carbon materials modulates physical properties for advanced applications in electronics, spintronics, and energy storage.
• High-pressure synthesis from multi-layer graphene often involves interfacial chemical transformations with pressure-transmitting media.
• Experimental characterization of molecular-scale interfacial mechanisms is challenging, and prior computational studies used simplified models lacking complexity and finite-temperature effects.

Purpose of the Study:

• To conduct an extensive computational study of bilayer graphene-methanol interfaces under high pressure and finite temperature.
• To provide fundamental insights into the structural, electronic, and reactivity properties of these complex interfaces.
• To address questions raised by previous experimental investigations.

Main Methods:

• Utilized advanced computational simulations on complex, realistic models of bilayer graphene-methanol interfaces.
• Employed state-of-the-art enhanced sampling techniques.
• Incorporated topological electronic descriptors for analysis.

Main Results:

• Characterized barrier-activated functionalization processes at the interface.
• Unveiled a significant catalytic effect of carbon defects and pressure on sp3 hybridization formation.
• Provided detailed insights into the structural and electronic properties under high-pressure conditions.

Conclusions:

• Carbon defects and high pressure are crucial catalysts for the functionalization of bilayer graphene with methanol.
• The findings offer a deeper understanding of interfacial mechanisms in 2D carbon materials synthesis.
• This work paves the way for designing novel carbon-based materials with tailored properties for technological applications.