Laser-induced enhancement of vertical polarization in ferroelectric bilayer WTe2

Abstract

Abstract 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 WTe2 by our real-time time-dependent density functional theory simulations. It is noted that bilayer WTe2 is 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.