Facet-dependent Chemical Kinetics Governed Growth of Twisted Graphene Layers with Pre-designed Angles

TL;DR

This paper presents a scalable chemical vapor deposition method to grow twisted graphene layers with pre-designed angles on platinum, using substrate engineering and understanding of growth kinetics.

Contribution

It introduces a substrate-engineering framework for controlling twist angles in graphene layers by manipulating platinum grain orientations during CVD growth.

Findings

Identified the activity sequence of Pt grains affecting graphene growth.

Revealed the role of surface morphology in graphene orientation.

Demonstrated programmable growth of TGLs with specific twist angles.

Abstract

Twisted graphene layers (TGLs) provide a powerful platform for investigating multiple quantum phenomena, yet their scalable deployment is hindered by the lack of reliable synthesis with precise angle. Here, benefited from a deeper understanding of the interplay between grain index and graphene growth kinetics, we report a scalable strategy to grow TGLs with pre-designed twist angles on platinum (Pt) via chemical vapor deposition (CVD), Through a combination of complementary in situ methods, we identified the activity sequence of different Pt grains and attributed it to the area ratio of exposed (110) facets during graphene-induced surface reconstruction. Moreover, we revealed that CVD-grown graphene orientation is determined by the grain-orientation-dependent surface morphology. By leveraging the so-established correlations between grain index with both graphene growth priority and its orientation, we achieve controlled folding and tearing of graphene overlayer using a pair of adjacent grains with dramatically different catalytical activity and kink-free atomic steps. We reveal that overlayer-induced step bunching and terrace reconfiguration critically govern the domain morphology and folding direction. Building on this mechanistic insight, we demonstrate a substrate-engineering framework where specific platinum grains are rationally selected to yield TGLs with pre-designed twist angles, including magic angle with flat band dispersion. This work not only highlights fundamental kinetics of Pt catalyzed graphene CVD growth, but also offers a generalizable methodology for manipulating foldable two-dimensional materials via dynamic substrate reconstruction, exampled by programmable growth of high-quality TGLs on open surfaces.