Antiferromagnetism-induced second-order nonlinear optical responses of centrosymmetric bilayer CrI3

Abstract

Antiferromagnetism (AF) in AB′-stacked centrosymmetric bilayer (BL) CrI3 breaks both spatial inversion (P) and time-reversal (T) symmetries but maintains the combined PTsymmetry, thus inducing novel second-order nonlinear optical (NLO) responses such as second-harmonic generation (SHG), linear electric-optic effect (LEO) and bulk photovoltaic effect (BPVE). In this work, we calculate AF-induced NLO responses of the BL CrI3 based on the density functional theory with the generalized gradient approximation (GGA) plus onsite Coulomb correlation (U), i.e., the GGA+U method. Interestingly, we find that the magnetic SHG, LEO and photocurrent in the AF BL CrI3 are huge, being comparable or even larger than that of the well-known nonmagnetic noncentrosymmetric semiconductors. For example, the calculated SHG coefficients are in the same order of magnitude as that of MoS2 monolayer (ML), the most promising 2D material for NLO devices. The calculated LEO coefficients are almost three times larger than that of MoS2 ML. The calculated NLO photocurrent in the CrI3BL is among the largest values predicted so far for the BPVE materials. On the other hand, unlike nonmagnetic semiconductors, the NLO responses in the AF BL CrI3 are nonreciprocal and also switchable by rotating magnetization direction. Therefore, our interesting findings indicate that the AF BL CrI3 will not only provide a valuable platform for exploring new physics of low-dimensional magnetism but also have promising applications in magnetic NLO and LEO devices such as frequency conversion, electro-optical switches, and light signal modulators as well as high energy conversion efficiency photovoltaic solar cells.