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We report structural, susceptibility and specific heat studies ofstoichiometric and off-stoichiometric poly- and single crystals of the A-sitespinel compound FeSc2S4. In stoichiometric samples no long-range magnetic orderis found down to 1.8 K. The magnetic susceptibility of these samples is fieldindependent in the temperature range 10 - 400 K and does not show irreversibleeffects at low temperatures. In contrast, the magnetic susceptibility ofsamples with iron excess shows substantial field dependence at hightemperatures and manifests a pronounced magnetic irreversibility at lowtemperatures with a difference between ZFC and FC susceptibilities and amaximum at 10 K reminiscent of a magnetic transition. Single crystal x-raydiffraction of the stoichiometric samples revealed a single phase spinelstructure without site inversion. In single crystalline samples with Fe excessbesides the main spinel phase a second ordered single-crystal phase wasdetected with the diffraction pattern of a vacancy-ordered superstructure ofiron sulfide, close to the 5C polytype Fe9S10. Specific heat studies reveal abroad anomaly, which evolves below 20 K in both stoichiometric andoff-stoichiometric crystals. We show that the low-temperature specific heat canbe well described by considering the low-lying spin-orbital electronic levelsof Fe2+ ions. Our results demonstrate significant influence of excess Fe ionson intrinsic magnetic behavior of FeSc2S4 and provide support for thespin-orbital liquid scenario proposed in earlier studies for the stoichiometriccompound.

Structure, magnetic susceptibility and specific heat of the spin-orbital-liquid candidate FeSc2S4 : Influence of fe off-stoichiometry