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We theoretically investigate the mechanism of ferroelectric switching via interlayer shear in 3R MoS 2  using first principles and lattice dynamics calculations. First principle calculations show the prominent anharmonic coupling of the infrared inactive interlayer shear and the infrared active phonons. The nonlinear coupling terms generates an effective anharmonic force which drives the interlayer shear mode and lowers the ferroelectric switching barrier depending on the amplitude and polarization of infrared mode. Lattice dynamics simulations show that the interlayer shear mode can be coherently excited to the switching threshold by a train of infrared pulses polarized along the zigzag axis of MoS 2 . The results of this study indicate the possibility of ultrafast ferroelectricity in stacked two-dimensional materials from the control of stacking sequence.

Ferroelectric switching in bilayer 3R MoS2 via interlayer shear mode driven by nonlinear phononics