Deformation-Potential-Driven Photostriction in Layered Ferroelectrics.

The coupling between electronic excitations and lattice deformation in van der Waals ferroelectrics is governed by a competition between the electron deformation potential and the inverse piezoelectric effect. While theory predicts that piezoelectric screening should drive a polar-axis contraction in monolayer group-IV monochalcogenides, we demonstrate that, in multilayer tin monosulfide (SnS), the deformation potential provides the dominant contribution, driving a polar-axis expansion even within ferroelectric domains. By correlating polarization-resolved second-harmonic generation microscopy with ultrafast reflectance spectroscopy and first-principles calculations, we resolve the anisotropic lattice response and disentangle intrinsic photostrictive strain from extrinsic thin-film interference artifacts. These results establish a microscopic hierarchy of photostrictive mechanisms and position stacking-engineered SnS as a platform for ultrafast optomechanical transduction.