Spatial anisotropy of the quantum spin liquid system YbMgGaO revealed by ab initio calculations.

YbMgGaO was recently proposed as a promising quantum-spin-liquid candidate material. However, some details of its structure, such as those related to a spatial anisotropy, were not completely understood. In this work, we perform ab initio calculations based on density-functional-theory to investigate the structural, the electronic and the magnetic properties of YbMgGaO. The geometrical model was constructed to take into account disorder effects produced by the random distribution of Ga and Mg along the lattice. We found a substantial spatial anisotropy revealed by variations up to 8% in the Mg-O and Ga-O bond lengths, which results in variations up to 3% in the Yb-Yb distances along its triangular lattice. Thus, the Yb lattice was not perfectly triangular. Furthermore, we demonstrate an out-of-plane magnetization at the Yb atoms with magnetic anisotropy energy of [Formula: see text] eV/Yb and a small interlayer exchange of [Formula: see text] eV/Yb, demonstrating that the system is only approximately two-dimensional. The presented results provide insights for an atomic-scale understanding of YbMgGaO with density-functional-theory calculations.