Abstract
BiFeO(3) has attracted great interest for its multiferroic property. The spontaneous electric polarization, multiferroism, and static magnetoelectric coupling have been widely studied both experimentally and theoretically. Here, in this paper, we report on the effects of magnetic ordering, spin fluctuation, and external magnetic field on the linear dielectric function and second-harmonic generation (SHG) in multiferroic BiFeO(3). First, our generalized gradient approximation plus Hubbard U calculations reproduce very well experimental data of linear dielectric function. In the mean time, it is revealed that SHG susceptibilities differ dramatically between antiferromagnetic configuration and ferromagnetic one, which is due to the enhanced contrast in the double-photon resonance absorption. Further Monte Carlo simulation of the coupling between electric order and spin-pair correlation function is presented for the spin fluctuation dependence of SHG. The significant nonlinear optical magnetoelectric effect around the Neel temperature provides novel route to enhancing magnetoelectric coupling in multiferroic materials.
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