Effect of entropy evolution on strongly correlated functionalities in charge-ordered manganites

The field of high entropy oxides (HEOs) flips the traditional paradigm of materials science, and the high configurational disorder endowing them with the potential for tailorable functional properties. In this work, the entropy-mediated phase stabilization concept is extended to charge-ordered manganite Pr1/2Ca1/2MnO3 to efficiently manipulate the physical properties. As specific amounts of trivalent (Nd and La) and divalent (Sr and Ba) elements are alternately doped into the manganite to form a single-phase solid solution, the system transitions from the spin-canted antiferromagnetic state to the ferromagnetic/antiferromagnetic alternating dominant state, and then further transitions to the ferrimagnetic-like state. The intense competition in magnetic exchange interactions leads to significant changes in temperature- and field-dependent resistance, highlighting the complex magneto-electronic phase diagram. The system also exhibits the coexistence of positive and negative magnetic entropy change and is significantly enhanced under specific doping conditions due to the metamagnetic phase transition. This study demonstrates that constructing stable strongly correlated manganites based on the entropy evolution design approach can effectively regulate various properties, providing opportunities to solve challenging problems in conventional systems.