Magnetoelectric Coupling at the Ni/Hf0.5Zr0.5O2 Interface

Composite multiferroics containing ferroelectric and ferromagnetic components often have much larger magnetoelectriccoupling compared to their single-phase counterparts. Doped or alloyed HfO2-based ferroelectrics may serve as apromising component in composite multiferroic structures potentially feasible for technological applications. Recently, astrong charge-mediated magnetoelectric coupling at the Ni/HfO2 interface has been predicted using density functional theorycalculations. Here, we report on the experimental evidence of such magnetoelectric coupling at the Ni/Hf0.5Zr0.5O2(HZO)interface. Using a combination of operando XAS/XMCD and HAXPES/MCDAD techniques, we probe element-selectively thelocal magnetic properties at the Ni/HZO interface in functional Au/Co/Ni/HZO/W capacitors and demonstrate clear evidence of the ferroelectric polarization effect on the magnetic response of a nanometer-thick Ni marker layer. The observed magnetoelectric effect and the electronic band lineup of the Ni/HZO interface are interpreted based on the results of our theoretical modeling. It elucidates the critical role of an ultrathin NiO interlayer, which controls the sign of the magnetoelectric effect as well as provides a realistic band offset at the Ni/HZO interface, in agreement with the experiment. Our results hold promise for the use of ferroelectric HfO2-based composite multiferroics for the design of multifunctional devices compatible with modern semiconductor technology.