Magnetism-induced second-order nonlinear optical responses in multiferroic BiFeO${}_3$

Abstract

Nonlinear optical (NLO) responses of noncentrosymmetric nonmagnets have drawn a lot of attention in the past decades because of their significance in materials characterization, green energy and device applications. However, the magnetism-induced NLO responses have rarely been studied so far. In this paper, we first extend the numerical calculation friendly formula by Rashkeev $\text{et al.}$ [Phys. Rev. B $\text{57}$, 3905 (1998)] for second harmonic generation (SHG) in nonmagnetic materials to include magnetic systems and then calculate the magnetism-induced NLO responses of BiFeO${}_3$, a multiferroic that exhibits both ferroelectricity and antiferromagnetic (AFM) ordering at room temperature and has a band gap that falls in the visible frequency region. First, we find that the calculated magnetism-induced SHG susceptibilities are large and the SHG intensity is tunable with the reversal of magnetization. In particular, we find a strong magnetic contrast of the SHG signal of approximately 440% at SHG photon energy of 4.82 eV, thus enabling a magnetic control of the SHG in BiFeO${}_3$. Also, because of the sensitivity of the SHG signal to the direction of the Néel vector, the SHG can be utilized to detect the reversal of the Néel vector in the AFM materials, which is an important issue for AFM spintronics. Second, the calculated BPVE in BiFeO${}_3$ are also strong, being larger than some well-known NLO compounds such as BaTiO${}_3$, GaAs, CdS and CdSe. Finally, we analyse the origins of the prominent features in the NLO response spectra in terms of the calculated quantum geometric quantities. Our interesting findings suggest that the magnetism-driven NLO responses in BiFeO${}_3$ are significant, anisotropic and tunable, and that understanding the magnetism-driven components of both SHG and BPVE is essential for their applications in, e.g., multiferroic-based photovoltaic devices.

References in corpus (11)

• First-principles study of spontaneous polarization in multiferroic BiFeO${}_3$
• Ferroelectric Materials for Solar Energy Conversion: Photoferroics Revisited
• Spectral and Fermi surface properties from Wannier interpolation
• Linear and Nonlinear Optical constants of BiFeO_3
• Nonlinear Optical Properties of Transition Metal Dichalcogenide MX${}_2$ (M = Mo, W; X = S, Se) Monolayers and Trilayers from First-principles Calculations
• Second-harmonic generation and linear electro-optical coefficients of SiC polytypes and nanotubes
• Large Second-Harmonic Generation and Linear Electro-Optic Effect in Trigonal Selenium and Tellurium
• First-Principles Studies of Second-Order Nonlinear Optical Properties of Organic-Inorganic Hybrid Halide Perovskites
• Large bulk photovoltaic effect and second-harmonic generation in few-layer pentagonal semiconductors PdS${}_2$ and PdSe${}_2$
• Tuning linear and nonlinear optical properties of wurtzite GaN by c-axial stress
• Antiferromagnetism-induced second-order nonlinear optical responses of centrosymmetric bilayer CrI${}_3$