Anomalous Gate-tunable Capacitance in Graphene Moiré Heterostructures

Interface engineered ferroelectricity in van der Waals heterostructures is of broad interest both fundamentally and technologically for the applications in neuromorphic computing and so on. In particular, the moiré ferroelectricity in graphene/hexagonal boron nitride (hBN) heterostructures driven by charge ordering instead of traditional lattice displacement has drawn considerable attention because of its fascinating properties and promising high-frequency programmable electrical polarization switching. Yet, the underlying mechanism of the electronic ferroelectricity is still under debate. On the other hand, combining the interface engineered ferroelectricity and strong correlations in moiré heterostructures could enable the realization of novel quantum states such as ferroelectric superconductivity and multiferroicity. Here we study the electronic transport properties of twisted double bilayer graphene (TDBLG), aligned with one of the neighbouring hBN. We observe a strong gating hysteresis and ferroelectric-like behaviour, as well as the electronic ratchet effect. We find that the top gate is anomalously screened. On the contrary, the back gate is anomalously doubly efficient in injecting charges into graphene, that is, the effective back gate capacitance is two times larger than its geometry capacitance. This unexpected gate-tunable capacitance causes a dramatic change of electric fields between forward and backward scans. The asymmetric gating behaviours and anomalous change in capacitance could be explained with a simple model involved with a spontaneous electric polarization between top hBN and graphene. Our work provides more insights into the mysterious ferroelectricity in graphene/hBN moiré heterostructures and paves the way to the understanding of the underlying mechanism.