Structure of twisted and buckled bilayer graphene

TL;DR

This study uses large-scale atomistic simulations to analyze the atomic structure of twisted bilayer graphene at very small mismatch angles, revealing vortex convergence, altered energy behavior, and significant buckling affecting its electronic properties.

Contribution

It introduces a computationally efficient simulation approach combining semi-empirical and interlayer potentials to study large twisted bilayer graphene samples at small angles.

Findings

Vortices in Moiré patterns converge to a constant size in the thermodynamic limit.

Energy behavior deviates from sinusoidal at angles below 1°.

Significant buckling occurs after relaxation, proportional to system size.

Abstract

We study the atomic structure of twisted bilayer graphene, with very small mismatch angles ($\theta \sim 0.28^0$), a topic of intense recent interest. We use simulations, in which we combine a recently presented semi-empirical potential for single-layer graphene, with a new term for out-of-plane deformations, [Jain et al., J. Phys. Chem. C, 119, 2015] and an often-used interlayer potential [Kolmogorov et al., Phys. Rev. B, 71, 2005]. This combination of potentials is computationally cheap but accurate and precise at the same time, allowing us to study very large samples, which is necessary to reach very small mismatch angles in periodic samples. By performing large scale atomistic simulations, we show that the vortices appearing in the Moir\'e pattern in the twisted bilayer graphene samples converge to a constant size in the thermodynamic limit. Furthermore, the well known sinusoidal behavior of energy no longer persists once the misorientation angle becomes very small ($\theta<1^0$). We also show that there is a significant buckling after the relaxation in the samples, with the buckling height proportional to the system size. These structural properties have direct consequences on the electronic and optical properties of bilayer graphene.