Atypical Sliding and Moiré Ferroelectricity in Pure Multilayer Graphene

Most nonferroelectric two-dimensional materials can be endowed with so-called sliding ferroelectricity via nonequivalent homobilayer stacking, which is not applicable to monoelement systems like pure graphene bilayer with inversion symmetry at any sliding vector. Herein, we show first-principles evidence that multilayer graphene with N>3 can all be ferroelectric, where the polarizations of polar states stem from the symmetry breaking in stacking configurations of across layer instead of adjacent layer, which are electrically switchable via interlayer sliding. The nonpolar states can also be electrically driven to polar states via sliding, and more diverse states with distinct polarizations will emerge in more layers. In contrast to the ferroelectric moiré domains with opposite polarization directions in twisted bilayers reported previously, the moiré pattern in some multilayer graphene systems (e.g., twisted monolayer-trilayer graphene) possess nonzero net polarizations with domains of the same direction separated by nonpolar regions, which can be electrically reversed upon interlayer sliding. The distinct moiré bands of two polar states should facilitate electrical detection of such sliding moiré ferroelectricity during switching.