Colossal magnetoresistance is of great fundamental and technological significance in condensed-matter physics, magnetic memory, and sensing technologies. However, its relatively narrow working temperature window is still a severe obstacle for potential applications due to the nature of the material-inherent phase transition. Here, we realized hierarchical LaSrMnO thin films with well-defined (001) and (221) crystallographic orientations by combining substrate modification with conventional thin-film deposition. Microscopic investigations into its magnetic transition through electron holography reveal that the hierarchical microstructure significantly broadens the temperature range of the ferromagnetic-paramagnetic transition, which further widens the response temperature range of the macroscopic colossal magnetoresistance under the scheme of the double-exchange mechanism. Therefore, this work puts forward a method to alter the magnetic transition and thus to extend the magnetoresistance working window by nanoengineering, which might be a promising approach also for other phase-transition-related effects in functional oxides.
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