New radical cation salt κ-(BETS)2Co0.13Mn0.87[N(CN)2]3 with two magnetic metals: Synthesis, structure, conductivity and magnetic peculiarities

•Magnetic doping: 13% of spin-5/2 Mn is replaced with spin-3/2 Co in κ‐(BETS)2Mn[N(CN)2]3.•Minor effect of the doping on crystal and band structure and conduction properties.•Dramatic effect of the doping on the magnetic anisotropy.•Potentiality to design different combinations of magnetic and conducting properties.

A new metallic radical cation salt κ‐(BETS)2Co0.13Mn0.87[N(CN)2]3, where BETS is bis(ethylenedithio)tetraselenafulvalene, C10S4Se4H8, has been synthesized. In this salt, a part of Mn2+ ions are replaced by Co2+ which acts as a magnetic dopant with a different effective magnetic moment. Crystal structure, band structure, conducting and magnetic properties of the salt have been studied. Below 30 K the material undergoes a metal-insulator transition, which is suppressed by applying a pressure of ∼0.5 kbar, leading to a superconducting ground state. While the structural and conducting properties are very similar to those of the parent salt κ‐(BETS)2Mn[N(CN)2]3, magnetic properties associated with localized moments in the anion layer are found to be surprisingly different.

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