Abstract

The electronic and magnetic structures ofFe1−xCuxCr2S4 (0.1≤x≤0.5) spinel sulfides have been investigated systematically by performingphotoemission spectroscopy (PES), soft x-ray absorption spectroscopy(XAS), and soft x-ray magnetic circular dichroism (XMCD) measurementsusing synchrotron radiation. Cr and Cu ions are found to be nearly trivalent(Cr3+) andmonovalent (Cu+), respectively, and their valence states do not change withx. The Fe 2pXAS spectra of Fe1−xCuxCr2S4 are very similar to that of Fe metal, indicating that the Fe 3d electrons are stronglyhybridized to other valence electrons. The Fe and Cr 2p XMCD spectra show thatthe magnetic moments of Cr ions and Fe ions are aligned antiparallel to eachother and that both the Cr and Fe magnetic moments increase with increasingx. The valence-band PES study reveals that theCr3+ () 3d states are located at ∼1.5 eV below EF. The occupied Fe 3d states consist of the broad states, the states at ∼4 eV below EF, and the states very close to EF. The filled Cu 3d10 states lie at ∼2.5 eV below EF. This study suggests that the hybridized Fe and S 3p states near EF play an important role in determining the transport properties ofFe1−xCuxCr2S4 for x≤0.5.

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