Ab initio determination of magnetic ground state of pyrochlore Y$_2$Mn$_2$O$_7$

TL;DR

This study uses ab initio calculations and simulations to determine that Y$_{2}$Mn$_{2}$O$_{7}$ has a ferromagnetic ground state, resolving previous experimental discrepancies and highlighting the role of orbital degrees of freedom in pyrochlore systems.

Contribution

It provides the first ab initio evidence that Y$_{2}$Mn$_{2}$O$_{7}$ is ferromagnetic, clarifying its magnetic ground state and exploring the influence of orbital degrees of freedom.

Findings

Y$_{2}$Mn$_{2}$O$_{7}$ has a ferromagnetic ground state.

Orbital degrees of freedom are key in the spin-glass behavior of Y$_{2}$Mo$_{2}$O$_{7}$.

Y$_{2}$Mn$_{2}$O$_{7}$ exhibits a single stable orbital configuration.

Abstract

There are two discrepant experimental results on the magnetic ground state of Y$_{2}$Mn$_{2}$O$_{7}$, one study proposes a spin glass state, while another introduces the material as a ferromagnet. In this study, we attempt to resolve this issue by employing density functional theory and Monte Carlo simulations. We derive different spin models by varying the Hubbard $U$ parameter in ab initio GGA+$U$ calculations. For the most range of Hubbard $U$, We obtain that the leading terms in the spin Hamiltonian are bi-quadratic and the nearest neighbor Heisenberg exchange interactions. By comparing Monte Carlo simulations of these models with the experiments, we find a ferromagnetic ground state for Y$_{2}$Mn$_{2}$O$_{7}$ as the most compatible with experiments. We also consider Y$_{2}$Mo$_{2}$O$_{7}$ as a prototype of the defect-free pyrochlore system with spin-glass behavior and compare it with Y$_{2}$Mn$_{2}$O$_{7}$. The orbital degrees of freedom are considered as a leading factor in converting a defect-free pyrochlore such as Y$_{2}$Mn$_{2}$O$_{7}$ to a spin glass system. By changing the $d$ orbital occupations of Mo atoms, our GGA+$U$ calculations for Y$_{2}$Mo$_{2}$O$_{7}$ indicate many nearly degenerate states with different $d$ orbital orientations which reveals $d$ orbital degrees of freedom in this material. While for Y$_{2}$Mn$_{2}$O$_{7}$, we find a single ground state with a fixed orbital orientation. Consequently, all of our ab initio approaches confirm Y$_{2}$Mn$_{2}$O$_{7}$ as a ferromagnetic system.