Most
previous attempts on achieving electric-field manipulation
of ferromagnetism in complex oxides, such as La0.66Sr0.33MnO3 (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.