Magnetic ordering induced giant optical property change in tetragonal BiFeO3

Magnetic ordering could have significant influence on band structures, spin-dependent transport, and other important properties of materials. Its measurement, especially for the case of antiferromagnetic (AFM) ordering, however, is generally difficult to be achieved. Here we demonstrate the feasibility of magnetic ordering detection using a noncontact and nondestructive optical method. Taking the tetragonal BiFeO3 (BFO) as an example and combining density functional theory calculations with tight-binding models, we find that when BFO changes from C1-type to G-type AFM phase, the top of valance band shifts from the Z point to Γ point, which makes the original direct band gap become indirect. This can be explained by Slater-Koster parameters using the Harrison approach. The impact of magnetic ordering on band dispersion dramatically changes the optical properties. For the linear ones, the energy shift of the optical band gap could be as large as 0.4 eV. As for the nonlinear ones, the change is even larger. The second-harmonic generation coefficient d33 of G-AFM becomes more than 13 times smaller than that of C1-AFM case. Finally, we propose a practical way to distinguish the two AFM phases of BFO using the optical method, which is of great importance in next-generation information storage technologies.