Quantum order by disorder is a key to understanding the magnetic phases of BaCo2(AsO4)2

Abstract

BaCo₂(AsO₄)₂ (BCAO), a honeycomb cobaltate, is considered a promising candidate for materials displaying the Kitaev quantum spin liquid state. This assumption is based on the distinctive characteristics of Co²⁺ ions (3d⁷) within an octahedral crystal environment, resulting in spin-orbit-coupled J_eff = 1/2 doublet states. However, recent experimental observations and theoretical analyses have raised questions regarding this hypothesis. Despite these uncertainties, reports of continuum excitations reminiscent of spinon excitations have prompted further investigations. In this study, we explore the magnetic phases of BCAO under both in-plane and out-of-plane magnetic fields, employing dc and ac magnetic susceptibilities, capacitance, and torque magnetometry measurement. Our results affirm the existence of multiple field-induced magnetic phases, with strong anisotropy of the phase boundaries between in-plane and out-of-plane fields. To elucidate the nature of these phases, we develop a minimal anisotropic exchange model. This model, supported by combined first principles calculations and theoretical modeling, quantitatively reproduces our experimental data. In BCAO, the combination of strong bond-independent XXZ anisotropy and geometric frustration leads to significant quantum order by disorder effects that stabilize colinear phases under both zero and finite magnetic fields.