Origin of magnetic frustration in Bi$_3$Mn$_4$O$_{12}$(NO$_3$)

Abstract

Bi$_3$Mn$_4$O$_{12}$(NO$_3$) (BMNO) is a honeycomb bilayers anti-ferromagnet, not showing any ordering down to very low temperatures despite having a relatively large Curie-Weiss temperature. Using ab initio density functional theory, we extract an effective spin Hamiltonian for this compound. The proposed spin Hamiltonian consists of anti-ferrimagnetic Heisenberg terms with coupling constants ranging up to third intra-layer and fourth inter-layer neighbors. Performing Monte Carlo simulation, we obtain the temperature dependence of magnetic susceptibility and so the Curie-Weiss temperature and find the coupling constants which best matches with the experimental value. We discover that depending on the strength of the interlayer exchange couplings, two collinear spin configurations compete with each other in this system. Both states have in plane N{\'e}el character, however, at small interlayer coupling spin directions in the two layers are antiparallel (N$_1$ state) and discontinuously transform to parallel (N$_2$ state) by enlarging the interlayer couplings at a first order transition point. Classical Monte Carlo simulation and density matrix renormalization group calculations confirm that exchange couplings obtained for BMNO are in such a way that put this material {at the phase boundary of a first order phase transition}, where the trading between these two collinear spin states prevents it from setting in a magnetically ordered state.