Ab initio investigation of the exchange interactions in Bi$_2$Fe$_4$O$_9$: The Cairo pentagonal lattice compound

TL;DR

This study uses ab initio calculations to analyze the complex exchange interactions in Bi$_2$Fe$_4$O$_9$, revealing a more intricate magnetic model than the ideal Cairo pentagonal lattice and explaining the observed orthogonal magnetic configuration.

Contribution

The paper provides the first ab initio calculation of exchange interactions in Bi$_2$Fe$_4$O$_9$, highlighting the need for a more complex model beyond the ideal Cairo lattice.

Findings

Identified five exchange parameters with specific values.

Showed that the dominant exchange ratios predict the orthogonal magnetic state.

Demonstrated the necessity of a more complex model for accurate description.

Abstract

We present the \emph{ab initio} calculation of the electronic structure and magnetic properties of Bi$_2$Fe$_4$O$_9$. This compound crystallizes in the orthorhombic crystal structure with the Fe$^{3+}$ ions forming the Cairo pentagonal lattice implying strong geometric frustration. The neutron diffraction measurements reveal nearly orthogonal magnetic configuration, which at first sight is rather unexpected since it does not minimize the total energy of the pair of magnetic ions coupled by the Heisenberg exchange interaction. Here we calculate the electronic structure and exchange integrals of Bi2Fe4O9 within the LSDA+U method. We obtain three different in-plane (J3=36 K, J4=73 K, J5=23 K) and two interplane (J1=10 K, J2=12 K) exchange parameters. The derived set of exchange integrals shows that the realistic description of Bi2Fe4O9 needs a more complicated model than the ideal Cairo pentagonal lattice with only two exchange parameters in the plane. However, if one takes into account only two largest exchange integrals, then according to the ratio x\equiv J3/J4=0.49<\sqrt{2} (a critical parameter for the ideal Cairo pentagonal lattice, see. Ref.~1) the ground state should be the orthogonal magnetic configuration in agreement with experiment. The microscopic origin of different exchange interactions is also discussed.