Origins of Graphite Resistivity: Decoupling Stacking Fault and Rotational Misorientation

ABSTRACT Van der Waals (vdW) layered materials, distinguished by weak interlayer interactions and diverse electronic properties, have ignited widespread research in materials science, physics, and device engineering. Interfacial dislocations, such as stacking faults (SF) and rotational misorientations (RM), are typically unavoidable and play a key role in shaping their interlayer transport properties. However, the absence of techniques to decouple their individual contributions has hindered a quantitative understanding of how stacking states affect interlayer electrical transport, even in well‐studied materials like graphite. In this work, we measure the intrinsic c‐axis resistivity of AB‐stacked epitaxial single‐crystal graphite (5.7 × 10 ⁻⁵ Ω · m) through high‐throughput measurements at room temperature. We further develop a decoupling strategy that combines rotational locking of highly oriented pyrolytic graphite (HOPG) with in situ measurements. Comparative analysis enable us to quantify, for the first time, the interlayer effective resistivity ratio of RM:SF:AB stacking as approximately 4507:74:1. In addition, we extend our methodology by introducing a large‐scale, pixel‐array‐based lateral measurement technique that reveals the internal dislocation structures and their tunability in vdW materials from a new spatial perspective. This work marks a significant advance in elucidating graphite's c‐axis electrical transport, providing a robust framework for investigating vdW materials with complex stacking structures.