Twisted two-dimensional van der Waals (vdW) heterostructures have unlocked a new means for manipulating the properties of quantum materials. The resulting mesoscopic moiré superlattices are accessible to a wide variety of scanning probes. To date, spatially-resolved techniques have prioritized electronic structure visualization, with lattice response experiments only in their infancy. Here, we therefore investigate lattice dynamics in twisted layers of hexagonal boron nitride (hBN), formed by a minute twist angle between two hBN monolayers assembled on a graphite substrate. Nano-infrared (nano-IR) spectroscopy reveals systematic variations of the in-plane optical phonon frequencies amongst the triangular domains and domain walls in the hBN moiré superlattices. Our first-principles calculations unveil a local and stacking-dependent interaction with the underlying graphite, prompting symmetry-breaking between the otherwise identical neighboring moiré domains of twisted hBN.

Moiré superlattices in van der Waals (vdW) heterostructures have given rise to a number of emergent electronic phenomena due to the interplay between atomic structure and electron correlations. A lack of a simple way to characterize moiré superlattices has impeded progress in the field. In this work we outline a simple, room-temperature, ambient method to visualize real-space moiré superlattices with sub-5 nm spatial resolution in a variety of twisted vdW heterostructures including but not limited to conducting graphene, insulating boron nitride and semiconducting transition metal dichalcogenides. Our method utilizes piezoresponse force microscopy, an atomic force microscope modality which locally measures electromechanical surface deformation. We find that all moiré superlattices, regardless of whether the constituent layers have inversion symmetry, exhibit a mechanical response to out-of-plane electric fields. This response is closely tied to flexoelectricity wherein electric polarization and electromechanical response is induced through strain gradients present within moiré superlattices. Moiré superlattices of 2D materials thus represent an interlinked network of polarized domain walls in a non-polar background matrix.