Much effort has been devoted recently to designing systems exhibiting simultaneous magnetic and ferroelectric
order (multiferroics) with a strong magnetoelectric coupling, which could enable the electrostatic control of magnetism
in the solid state. One approach consists of exploring interfacial couplings between magnetic and ferroelectric
phases of composite systems, where magnetoelectric couplings larger than those typical of single-phase multiferroics
have been achieved. Here, we overview our recent work on epitaxial Pb(Zr0.2Ti0.8)O3/La0.8Sr0.2MnO3
(PZT/LSMO) heterostructures tailored to display a large magnetoelectric coupling, which relies on the sensitivity
of the magnetic properties of the doped manganites to charge. The magnetoelectric response in this system
is hysteretic, displaying abrupt switching between two magnetic states for the two states of the ferroelectric
polarization. The microscopic origin of this effect, which is studied using advanced spectroscopic techniques,
arises from changes of the valence state of Mn in LSMO induced by the electrostatic modulation in the charge
carrier density. Hence, the magnetoelectric coupling in these multiferroic heterostructures is charge-based and
electronic in origin. From a quantitative comparison between the measured change in valency and magnetic
moment, we conclude that the interfacial spin ordering is modified upon charge doping. This ability to control
spin via electric fields opens a new pathway for the development of novel spin-based technologies.
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