Ultrafast near-infrared nonlinear absorption in a multiferroic single crystal of bismuth ferrite

Abstract

We studied the ultrafast third-order optical nonlinearity in a single crystal of multiferroic bismuth ferrite (BiFeO3) in the near-infrared range of 0.5–1.0 eV, where the material is fundamentally transparent, at room temperature. With pump pulses at 1.55 eV, which is off-resonant to the strong inter-band charge transfer (CT) transition, we observed instantaneous transient absorption with a pencil-like temporal profile originating from the two-photon CT transition from the oxygen 2p to the iron 3d levels. In contrast, under pumping with 3.10 eV photons, the pencil-like absorption change was not observed but decay profiles showed longer time constants. Although the two-photon absorption coefficient estimated to be 1.5 cm/GW is 10 (100) times smaller than that of two (one)-dimensional cuprates, it is larger than those of common semiconductors such as ZnSe at the optical communication wavelength.