Antiferromagnetism-induced second-order nonlinear optical responses of centrosymmetric bilayer CrI${}_3$

Abstract

Antiferromagnetism (AF) in AB'-stacked centrosymmetric bilayer (BL) CrI${}_3$ breaks both spatial inversion ($P$) and time-reversal ($T$) symmetries but maintains the combined $PT$ symmetry, 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 CrI${}_3$ 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 CrI${}_3$ 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 MoS${}_2$ monolayer (ML), the most promising 2D material for NLO devices. The calculated LEO coefficients are almost three times larger than that of MoS${}_2$ ML. The calculated NLO photocurrent in the CrI${}_3$ BL 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 CrI${}_3$ are nonreciprocal and also switchable by rotating magnetization direction. Therefore, our interesting findings indicate that the AF BL CrI${}_3$ 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.

arXiv comment10 pages, 7 figures

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• Large bulk photovoltaic effect and second-harmonic generation in few-layer pentagonal semiconductors PdS${}_2$ and PdSe${}_2$
• Classification of second harmonic generation effect in magnetically ordered materials
• Magnetism-induced second-order nonlinear optical responses in multiferroic BiFeO${}_3$