Yb${}^{3+}$ $f$-$f$ excitations in NaYbSe${}_2$: benchmarking embedded-cluster quantum chemical schemes for 4$f$ insulators

Abstract

$\tilde{S}=1/2$ triangular-lattice $f$-electron materials define a dynamic research area in condensed matter magnetism. In various Yb 4$f^{13}$ triangular-lattice compounds, for example, spin-liquid ground states seem to be realized. Using {\it ab initio} quantum chemical methods, we here investigate how correlation effects involving the 4$f$ electrons affect the on-site $f$-$f$ excitation spectrum in NaYbSe${}_2$. The system is well suited for such a study since unambiguous inelastic neutron scattering data are available for the Yb${}^{3+}$ $f$-$f$ transitions. The excitation energies obtained by configuration-interaction calculations with single and double substitutions agree within 3-4 meV with experimental values, which provides a not so expensive alternative to fitting experimental data at the model-Hamiltonian level in order to analyze $f$-center multiplet structures.

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