Trigonal distortion in the Kitaev candidate honeycomb magnet BaCo2(AsO4)2

Abstract

We conducted x-ray absorption (XAS) and magnetic circular dichroism (XMCD) measurements at the Co $L_{2,3}$ edges on single crystals of the Kitaev candidate honeycomb lattice compound BaCo$_2$(AsO$_4$)$_2$. The measurements employed the inverse partial fluorescence yield technique, which is ideal for acquiring reliable x-ray absorption spectra from highly insulating samples, enabling precise quantitative analysis. Our experimental results revealed a significant linear dichroic signal, indicating strong trigonal distortion in the CoO$_{6}$ octahedra in BaCo$_2$(AsO$_4$)$_2$. We performed a detailed analysis of the experimental XAS and XMCD spectra using a full-multiplet configuration-interaction cluster model. This analysis unveiled that the $t_{2g}$ hole density is predominantly localized in the $a_{1g}$ orbital. Through XMCD sum rules and theoretical calculations, we quantified both the spin and orbital magnetic moments. Our study demonstrates that the local electronic structure of the CoO$_{6}$ octahedra displays an effective trigonal distortion of approximately $-0.114$ eV. This distortion is larger than the Co $3d$ spin-orbit coupling constant, emphasizing the crucial impact of local structural distortions on the electronic and magnetic properties of BaCo$_2$(AsO$_4$)$_2$.