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Dynamic tuning of ion concentrations to create new functionalities in magnetoresistive La0.67Sr0.33MnO3 (LSMO) has attracted much attention. However, oxygen-vacancy-driven processes require extremely high temperatures (> 500oC) and take several days. Here, we found that by simply annealing platinum-dotted LSMO films in hydrogen and argon at the relatively low temperatures of 150–200oC for several minutes, we could achieve reversible changes in the resistivity over three orders of magnitude, with tailored ferromagnetic mag-netization. While oxygen-driven processes are usually accompanied by topotactic transitions between perovskite and brownmillerite, our reversible transition occurs in a perovskite. We suggest that this transition occurs due to electron-doping-induced modulation of double exchange interactions and/or lattice expansion, along with increases in the hydrogen concen-tration. Our findings offer high reproducibility, long-time stability, and linear multilevel ap-peal for ionotronic (ionic + electronic) applications.
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