Hydrogen Control of Double Exchange Interaction in La_0.67Sr_0.33MnO₃ for Ionic–Electric–Magnetic Coupled Applications

The dynamic tuning of ion concentrations has attracted significant attention for creating versatile functionalities of materials, which are impossible to reach using classical control knobs. Despite these merits, the following fundamental questions remain: how do ions affect the electronic bandstructure, and how do ions simultaneously change the electrical and magnetic properties? Here, by annealing platinum-dotted La_0.67Sr_0.33MnO₃ films in hydrogen and argon at a lower temperature of 200 °C for several minutes, a reversible change in resistivity is achieved by three orders of magnitude with tailored ferromagnetic magnetization. The transition occurs through the tuning of the double exchange interaction, ascribed to an electron-doping-induced and/or a lattice-expansion-induced modulation, along with an increase in the hydrogen concentration. High reproducibility, long-term stability, and multilevel linearity are appealing for ionic–electric–magnetic coupled applications.