Ultrafast Modulation of Stacking Orders in vdW Layers by Photoinduced Pseudosliding of Ferroelectric Monolayer.

Precise control of stacking orders in van der Waals (vdW) heterostructures not only generates novel quantum phenomena but also promises applications in memory and computing devices. However, achieving robust control of the stacking order in vdW heterostructures remains a significant challenge. In this work, TDDFT-MD simulations reveal a photoinduced ultrafast and nonvolatile in-plane structural transition in ferroelectric antimonene. This transition can modify the stacking order in vdW heterostructures based on antimonene. It resembles a sliding effect but retains the geometric center of the antimonene layer and is therefore termed pseudosliding. Furthermore, optical-property switching via pseudosliding is also demonstrated in an Sb/SnSe vdW heterostructure. The present work proposes a new strategy for ultrafast and robust control of stacking orders in vdW heterostructures, leveraging ferroelectric monolayers with an in-plane Peierls distortion.