Combined Experimental\nand Theoretical Approach to\nthe Electronic and Magnetic Properties of Cu-Doped LaMnO<sub>3</sub> Perovskites

Cu-doped LaCu<sub><i>x</i></sub>Mn<sub>1–<i>x</i></sub>O<sub>3</sub> perovskites have been used as a model\nsystem for a joint experimental and theoretical assessment of the\ninfluence of the Cu doping level on the structural, electronic, and\nmagnetic properties. The different Cu-doped phases LaCu<sub>0.3</sub>Mn<sub>0.7</sub>O<sub>3</sub> (LCM37), LaCu<sub>0.5</sub>Mn<sub>0.5</sub>O<sub>3</sub> (LCM55), and LaCu<sub>0.7</sub>Mn<sub>0.3</sub>O<sub>3</sub> (LCM73) including the respective Cu- and Mn-free benchmark\nmaterials La<sub>2</sub>CuO<sub>4</sub> (LC) and LaMnO<sub>3</sub> (LM) have been studied by magnetization measurements and electronic\nparamagnetic resonance. Ferromagnetic behavior was detected for pure\nLM and all Cu-doped perovskites, whereas antiferromagnetic behavior\nwas revealed for La<sub>2</sub>CuO<sub>4</sub>. Generally, an increased\nantiferromagnetic contribution was shown for higher Cu doping levels.\nEqually, magnetization was highlighted to decrease with increasing\nCu content. Sophisticated hybrid density functional theory calculations\nof the electronic and magnetic properties using defect-free, idealized\nCu-doped model structures agree well with the experimental results.\nThe findings reveal that copper incorporation influences both the\nelectronic conductivity and the magnetic properties. Notably, the\nmaterials exhibit a tunable degree of half-metallicity and significant\nelectronic spin polarization, establishing them as promising candidates\nfor advanced technological applications in spintronics and catalysis.\nThe insights gained from this study contribute to a broader understanding\nof perovskite materials and their versatile applications.