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We study the magnetic susceptibility of mixed-valent La2-xSrxCoO4 singlecrystals in the doping range of 0.5<= x <= 0.8 for temperatures up to 1000 K.The magnetism below room temperature is described by paramagnetic Co2+ in thehigh-spin state and by Co3+ in the non-magnetic low-spin state. Above roomtemperature, an increase in susceptibility compared to the behavior expectedfrom Co2+ is seen, which we attribute to a spin-state transition of Co3+. Thesusceptibility is analyzed by comparison to full-multiplet calculations for thethermal population of the high- and intermediate-spin states of Co3+.

Evidence for a temperature-induced spin-state transition of Co3+ in La2-xSrxCoO4