Laser-induced enhancement of vertical polarization in ferroelectric bilayer WTe₂

Light-matter interaction is one of the key means to manipulate the structural and electronic properties of materials, especially in two-dimensional (2D) layered materials, which are optically accessible due to their atomic thickness. We propose that an ultrashort laser pulse could drastically enhance the ferroelectric polarization of bilayer WTe₂by our real-time time-dependent density functional theory simulations. It is noted that bilayer WTe₂is a 2D sliding ferroelectric material recently discovered whose vertical polarization can be controlled by a slight horizontal displacement. We demonstrate that interlayer sliding and compression are simultaneously achieved upon illumination of linearly polarized near-infrared laser pulse, leading to an ultrafast electric polarization enhancement by ∼230% within hundreds of femtosecond. Two major contributions have been identified: (a) the piezoelectric effect due to laser-induced interlayer compression, caused by interlayer charge transfer and dipole-dipole interaction; (b) the interlayer sliding along the opposite direction of ferroelectric switching, induced by inhomogeneous excited carrier distribution and specific electron-phonon couplings. This work provides new insights on controlling ferroelectricity of layered materials, which may extend to other van der Waals bilayers and even bulk materials.