5d-mediated indirect exchange and effective spin Hamiltonians in Ce triangular-lattice delafossites

Abstract

Anisotropic intersite exchange interactions in frustrated rare-earth magnets are difficult to assess both theoretically and experimentally. Here, we propose an ab initio force-theorem framework combining the quasi-atomic Hubbard-I approach to 4f correlations with a static mean-field treatment of the on-site intershell Coulomb interaction between rare-earth 4f and 5d states to simultaneously capture both 4f superexchange and 5d-mediated indirect exchange. Applying it to the triangular lattice Ce delafossites CsCeSe${}_2$, KCeS${}_2$, and RbCeO${}_2$, we find that the indirect exchange dominates in the selenide, the superexchange in the oxide, while both mechanisms contribute almost equally in the sulfide. The magnetic exciation spectra of CsCeSe${}_2$ and KCeS${}_2$ evaluated from the calculated spin Hamiltonains are in good qualitative and quantitative agreement with experimental data.

Accepted version. 8 pages, 3 figures + 4 pages of Supplementary

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