Layer Decoupling in Twisted Bilayer WSe$_2$ Uncovered by Automated Dark-Field Tomography

Abstract: Twisted bilayer systems host a wealth of emergent phenomena, such as flat-band superconductivity, ferromagnetism, and ferroelectricity, arising from moiré superlattices and unconventional interlayer coupling. Despite their central role, direct and quantitative access to the out-of-plane atomic structure in these systems has remained elusive due to their nanoscale dimensions. Here, we introduce an automated dark-field electron tomography technique that enables three-dimensional structural analysis of atomically thin materials with sub-angstrom precision. Applying this method to twisted bilayer WSe$_2$, we uncover a significant expansion of the interlayer spacing compared to the bulk configuration, exceeding 0.1 angstrom, along with a remarkable temperature-driven interlayer decoupling unique to the twisted bilayer. Ultrafast measurement further reveals optically induced interlayer separation of ~0.2 angstrom on the picosecond timescale, attributed to transient exciton formation. These findings not only establish a powerful approach for visualizing hidden out-of-plane structures in atomically thin micro-flake materials, but also uncover the intrinsic fragility and dynamical tunability of interlayer coupling in moiré-engineered 2-dimensional materials.