Tuning Fe concentration in epitaxial gallium ferrite thin films for room temperature multiferroic properties

Abstract Stoichiometric gallium ferrite (GFO) is a promising single-phase multiferroic material at room temperature. Nevertheless, simultaneous magnetism and ferroelectricity in a single GFO at room temperature has not been demonstrated yet. In this work, single-phase GFO thin films with different amount of excessive Fe have been successfully grown using a dual target pulsed laser deposition (PLD) process, and the magnetic transition temperature is found to be above room temperature with excessive Fe distributed among the available cation sites of GFO unit cell. Ferroelectricity of GFO films have been confirmed by second harmonic generation (SHG), polarization hysteresis, pyroelectric reversal, and piezoresponse force microscopy (PFM), and magnetoelectric (ME) coupling has been demonstrated by increase in piezoresponse induced via external magnetic field applied in-plane, all measured at room temperature. From the data, it is theorized that the magnetic properties of GFO originate from the superexchange interaction mediated via the Fe1-O-Fe2 bond, and an additional Fe1-O-Fe* bond can form from excess Fe atoms. Under a magnetic field applied along c axis, the magnetic moment of Fe2 and Fe* increase while that of Fe1 decreases, and these changes in magnetic moment result in larger distortion of Fe2 and Fe* octahedrons along the b-axis, and thus enhanced polarization and piezoresponse. This series of studies thus confirm single-phase GFO with excessive Fe as a multiferroic material at room temperature with ME coupling, paving way for its potential functional applications in microelectronic and spintronic devices.