Spin-layer locking induced second-order nonlinear effect in centrosymmetric crystals

According to the generally accepted nonlinear principles, second-order nonlinear effect (SONE) is strongly inhibited by the crystalline symmetries and thus can manifest only in non-centrosymmetric materials with broken global spatial inversion symmetry. In stark contrast, here we report the observation of direct-current (DC) related SONE, including circular and linear photogalvanic effects, in centrosymmetric bilayer and multilayer MoS2. In conjunction with relativistic first-principles calculations, we uncover that the observed DC-related SONE in inversion-symmetric MoS2 results from the localized electronic states and the locking of spin with the layer and valley pseudospins. Our results provide a new insight into nonlinear physics and would be applicable to other phenomena thus far believed to occur only in non-centrosymmetric systems, such as quantum spin Hall effect, valley Hall effect, piezoelectricity and unconventional Ising superconductivity.