Quadratic piezoelectricity from stacking-engineered interference in multilayer sliding ferroelectrics

Abstract

Designing nonlinear piezoelectricity requires suppressing the linear piezoelectric coefficient without extinguishing higher-order electromechanical response, yet a general and reconfigurable route remains lacking. Here we introduce stacking-engineered piezoelectric interference as such a mechanism in multilayer sliding ferroelectrics. Combining first-principles calculations with a generalized Ginzburg--Landau framework, we show that each interlayer gap acts as a local piezoelectric channel whose sign and magnitude are determined by stacking. Constructive interference between same-signed channels produces a linear-dominated response, whereas destructive interference between oppositely signed channels suppresses the linear coefficient while preserving a finite quadratic response. Representative MoS$_2$ and NiTe$_2$ multilayers approach the parabolic limit, with BAAC-stacked MoS$_2$ reducing the linear-to-quadratic crossover strain by a factor of 25 relative to CBA-stacked MoS$_2$. Experimentally accessible tetralayer MoS$_2$ sliding pathways further connect linear-dominated, quadratic-dominated and sign-inverted states. Here, we identify stacking-engineered interference as a design principle for programmable nonlinear electromechanics in layered materials.