An Atomistic Insight into Moiré Reconstruction in Twisted Bilayer Graphene beyond the Magic Angle

[Image: see text] Twisted bilayer graphene exhibits electronic properties strongly correlated with the size and arrangement of moiré patterns. While rigid rotation of the two graphene layers results in a moiré interference pattern, local rearrangements of atoms due to interlayer van der Waals interactions result in atomic reconstruction within the moiré cells. Manipulating these patterns by controlling the twist angle and externally applied strain provides a promising route to tuning their properties. Atomic reconstruction has been extensively studied for angles close to or smaller than the magic angle (θ(m) = 1.1°). However, this effect has not been explored for applied strain and is believed to be negligible for high twist angles. Using interpretive and fundamental physical measurements, we use theoretical and numerical analyses to resolve atomic reconstruction in angles above θ(m). In addition, we propose a method to identify local regions within moiré cells and track their evolution with strain for a range of representative high twist angles. Our results show that atomic reconstruction is actively present beyond the magic angle, and its contribution to the moiré cell evolution is significant. Our theoretical method to correlate local and global phonon behavior further validates the role of reconstruction at higher angles. Our findings provide a better understanding of moiré reconstruction in large twist angles and the evolution of moiré cells under the application of strain, which might be potentially crucial for twistronics-based applications.