Hydrogenation driven structural transformation and adjustable electronic properties of epitaxial La0.3Sr0.7MnO3−δ films

Manganites (R1−xAxMnO3, R = rare-earth cation and A = alkali or alkaline earth cation) host an immense number of phases and electronic properties, which can be mainly manipulated through conventional structural control such as metallic cations, oxygen concentration, or misfit strain. However, their practical applications are heavily hindered due to the requirement of rigid synthesis conditions and prolonged treatment time. Herein, a subtle hydrogenation of canonical epitaxial La0.3Sr0.7MnO3 films gives rise to a series of structural transformations ranging from the perovskite to the intermediate state and to the brownmillerite one, accompanied by tunable electronic performances from the antiferromagnetic insulating phase to the weak magnetic insulating one. Moreover, the hydrogenated La0.3Sr0.7MnO3−δ films show an ultra-high magnetic temperature (>400 K). The efficient modulations of the crystalline structure and functionalities of manganite oxides using the facile hydrogenation process enable practical applications of high-temperature magnetic insulators in spintronic devices.