Magnetic Behavior of Volborthite Cu₃V₂O₇(OH)₂ * 2(H₂O) Determined by Coupled Trimers Rather than Frustrated Chains

Abstract

Motivated by recent experiments on volborthite single crystals showing a wide 1/3-magnetization plateau, we perform microscopic modeling by means of density functional theory (DFT) with the single-crystal structural data as a starting point. Using DFT+U, we find four leading magnetic exchanges: antiferromagnetic J and J2, as well as ferromagnetic J0 and J1. Simulations of the derived spin Hamiltonian show good agreement with the experimental low-field magnetic susceptibility and high-field magnetization data. The 1/3 -plateau phase pertains to polarized magnetic trimers formed by strong J bonds. An effective J -> infty model shows a tendency towards condensation of magnon bound states preceding the plateau phase.