Single-site magnetic anisotropy governed by inter-layer cation charge imbalance in triangular-lattice AYbX$_2$

TL;DR

This study reveals that inter-layer cation charge imbalance significantly influences the magnetic anisotropy of Yb$^{3+}$ ions in layered triangular-lattice materials, with implications for understanding spin-liquid candidates.

Contribution

It demonstrates that inter-layer charge imbalance, rather than ligand distortions, governs the anisotropic $g$ tensor in Yb-based layered compounds.

Findings

Inter-layer cation charge imbalance affects $g$ tensor anisotropy.

Less inter-layer positive charge enhances in-plane magnetic response.

Charge imbalance is a general feature in 4f$^{13}$ layered materials.

Abstract

The behavior in magnetic field of a paramagnetic center is characterized by its $g$ tensor. An anisotropic form of the latter implies different kind of response along different crystallographic directions. Here we shed light on the anisotropy of the $g$ tensor of Yb$^{3+}$ 4$f^{13}$ ions in NaYbS$_2$ and NaYbO$_2$, layered triangular-lattice materials suggested to host spin-liquid ground states. Using quantum chemical calculations we show that, even if the ligand-cage trigonal distortions are significant in these compounds, the crucial role in realizing strongly anisotropic, `noncubic' $g$ factors is played by inter-layer cation charge imbalance effects. The latter refer to the asymmetry experienced by a given Yb center due to having higher ionic charges at adjacent metal sites within the magnetic $ab$ layer, i.e., 3+ nearest neighbors within the ab plane versus 1+ species between the magnetic layers. According to our results, this should be a rather general feature of 4$f^{13}$ layered compounds: less inter-layer positive charge is associated with stronger in-plane magnetic response.