Chemical doping and epitaxy can be used to tailor the magnetoelectric properties of multiferroic thin films, such as SrMnO3. Here, we study the dependence of the magnetic order temperatures of Sr1−xBaxMnO3 thin films on epitaxial strain and Ba content. Combining low-energy muon spin spectroscopy and scanning transmission electron microscopy, the broadness of the magnetic transition is attributed to the presence of a Mn-O-Mn angle gradient along the out-of-plane direction. We also demonstrate that the unit cell volume is the key parameter to determine the Néel temperature in Sr1−xBaxMnO3 thin films showing G-type antiferromagnetic order. The occurrence of a simultaneously ferroelectric and ferromagnetic ground state at high strain levels is suggested for the Sr0.8Ba0.2MnO3 thin film deposited on TbScO3.
