Hard x-ray photoemission spectroscopy of the ferrimagnetic series Gd6(Mn1-xFex)23

T. Ly Nguyen, Th Mazet, D. Malterre, H. J. Lin, M. Yoshimura, Y. F. Liao, H. Ishii, N. Hiraoka, Y. C. Tseng, A. Chainani

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Abstract

We study the evolution of the electronic structure of the intermetallic series Gd6(Mn1-xFex)23, x=0.0-0.75, which shows nonmonotonic ferrimagnetic ordering temperatures TC but with a systematic reduction of the total bulk magnetization upon increasing Fe content, x. We have carried out hard x-ray photoemission spectroscopy to elucidate the relation between electronic structure and properties of the series. The Gd 3d and Gd 4d core-level spectra indicate trivalent Gd3+ multiplets in the intermediate-coupling scheme with features due to L-S and j-J coupling. The Fe 2p core levels show asymmetric single peak metal-like spectra, while the Mn 2p core levels show asymmetric doublet peaks. The relative intensities of the Mn 2p doublets as a function of x indicate occupancy changes of distinct crystallographic sites associated with Mn up-spin and down-spin states. The valence band spectra identify the Gd 4f states at high binding energies (∼7.4 eV). The Mn 3d states occur at the Fermi level and as a broad feature between 2 and 5 eV binding energy in Gd6Mn23. Upon substitution, the Fe 3d states show up as small shifts to higher binding energies compared to Mn 3d states. The Fe 3s and Mn 3s spectra show exchange split peaks, allowing an estimate of the Mn and Fe magnetic moments using a Van Vleck analysis, which also provides a quantification of occupancy changes with x. The overall results are consistent with the bulk net magnetization, indicating that Mn up-spin sites become Fe down-spin sites on substitution, while the nonmonotonic TC originates in a change from Mn sublattice to Fe sublattice derived ordering.

Original languageEnglish
Article number045144
JournalPhysical Review B
Volume106
Issue number4
DOIs
StatePublished - 15 Jul 2022

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