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

TL;DR

This study investigates the ultrafast optical nonlinearity of multiferroic bismuth ferrite in the near-infrared, revealing two-photon absorption mechanisms and their potential for optical applications.

Contribution

It provides the first detailed analysis of third-order nonlinear optical responses in BiFeO3 in the near-infrared range at room temperature.

Findings

Observed instantaneous transient absorption at 1.55 eV pump due to two-photon charge transfer.

Identified longer decay profiles with 3.10 eV pump, indicating different relaxation dynamics.

Measured two-photon absorption coefficient of 1.5 cm/GW, larger than common semiconductors.

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 pencil-like temporal profile originating from the two-photon CT transition from the oxygen 2p to the iron 3p 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 is estimated to be 1.5 cm/GW, which is ten (hundred) times smaller than that of two(one)-dimensional cuprates, it is larger than those of common semiconductors such as ZnSe and GaAs at the optical communication wavelength.