Multiscale analysis of large twist ferroelectricity and swirling dislocations in bilayer hexagonal boron nitride

Abstract: With its atomically thin structure and intrinsic ferroelectric properties, heterodeformed bilayer hexagonal boron nitride (hBN) has gained prominence in next-generation non-volatile memory applications. However, studies to date have focused almost exclusively on small heterodeformations, leaving the question of whether ferroelectricity can persist under large heterodeformation entirely unexplored. In this work, we establish the crystallographic origin of ferroelectricity in bilayer hBN configurations heterodeformed relative to high-symmetry configurations such as the AA-stacking and the 21.786789 $\circ$ twisted configuration, using Smith normal form bicrystallography. We then demonstrate out-of-plane ferroelectricity in bilayer hBN across configurations vicinal to both the AA and $\Sigma 7$ stacking. Atomistic simulations reveal that AA-vicinal systems support ferroelectricity under both small twist and small strain, with polarization switching in the latter governed by the deformation of swirling dislocations rather than the straight interface dislocations seen in the former. For $\Sigma 7$-vicinal systems, where reliable interatomic potentials are lacking, we develop a density-functional-theory-informed continuum framework--the bicrystallography-informed frame-invariant multiscale (BFIM) model, which captures out-of-plane ferroelectricity in heterodeformed configurations vicinal to the $\Sigma 7$ stacking. Interface dislocations in these large heterodeformed bilayer configurations exhibit markedly smaller Burgers vectors compared to the interface dislocations in small-twist and small-strain bilayer hBN. The BFIM model reproduces atomistic simulation results and provides a powerful, computationally efficient framework for predicting ferroelectricity in large-unit-cell heterostructures where atomistic simulations are prohibitively expensive.