Modulating Magnetism in Ferroelectric Polymer-Gated Perovskite Manganite Films with Moderate Gate Pulse Chains

Most previous attempts on achieving electric-field manipulation of ferromagnetism in complex oxides, such as La_0.66Sr_0.33MnO₃ (LSMO), are based on electrostatically induced charge carrier changes through high-k dielectrics or ferroelectrics. Here, the use of a ferroelectric copolymer, polyvinylidene fluoride with trifluoroethylene [P(VDF-TrFE)], as a gate dielectric to successfully modulate the ferromagnetism of the LSMO thin film in a field-effect device geometry is demonstrated. Specifically, through the application of low-voltage pulse chains inadequate to switch the electric dipoles of the copolymer, enhanced tunability of the oxide magnetic response is obtained, compared to that induced by ferroelectric polarization. Such observations have been attributed to electric field-induced oxygen vacancy accumulation/depletion in the LSMO layer upon the application of pulse chains, which is supported by surface-sensitive-characterization techniques, including X-ray photoelectron spectroscopy and X-ray magnetic circular dichroism. These techniques not only unveil the electrochemical nature of the mechanism but also establish a direct correlation between the oxygen vacancies created and subsequent changes to the valence states of Mn ions in LSMO. These demonstrations based on the pulsing strategy can be a viable route equally applicable to other functional oxides for the construction of electric field-controlled magnetic devices.