Emergent magnetism, heavy electrons and pressure-induced reentrant superconductivity in the iron substituted 4d transition-metal sulfides

Abstract

Superconductivity emerging from or in the vicinity of magnetic states is generally considered to be mediated by spin fluctuations and thus lies beyond the scope of conventional electron-phonon coupled BCS framework. Here we report the emergence of novel ferromagnetism in the d-electron rhodium sulfide Rh17S15 superconductor, characterized by an enhanced Sommerfeld coefficient γ arising from the flat topological band and many-body correlations. We further demonstrate that the ferromagnetism can be tuned via Fe substitution at the Rh sites, leading to a spin glass ground state induced by the competing ferromagnetic and antiferromagnetic exchange interactions. Fe doping results in a further enhancement of both the γ and electron effective masses. At a doping level of x = 0.67 in Rh17-xFexS15, γ reaches 312 mJ mol-1K-2, second only to the well-documented d-electron heavy-fermion material LiV2O4. Furthermore, upon applying pressure, superconductivity is first suppressed; under high pressures, however, we observe the reentrant superconductivity in both pristine and Fe-doped samples. Our results not only demonstrate the unusual magnetic states and possible heavy-fermion features in these frustration-free, d-based superconductors, but also suggest that the superconductivity in this system is likely mediated by the intrinsic spin fluctuations and may thus be unconventional.

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