Prediction of exotic magnetic states in the alkali metal quasi-one-dimensional iron selenide compound Na$_2$FeSe$_2$

TL;DR

This study predicts exotic magnetic states, including a block magnetic order, in the quasi-one-dimensional alkali metal iron selenide compound Na$_2$FeSe$_2$, using advanced theoretical modeling and numerical techniques.

Contribution

It introduces a first-principles derived model predicting novel magnetic phases, including a block state, in Na$_2$FeSe$_2$, a material with Fe$^{2+}$ valence, expanding understanding of magnetic order in iron selenides.

Findings

Identification of a stable block magnetic state in the phase diagram.

Prediction of a transition to a staggered spin order at high Hubbard repulsion.

Discovery of a mixed phase with inhomogeneous orbital and spin configurations.

Abstract

The magnetic and electronic phase diagram of a model for the quasi-one-dimensional alkali metal iron selenide compound Na$_2$FeSe$_2$ is presented. The novelty of this material is that the valence of iron is Fe$^{2+}$ contrary to most other iron-chain compounds with valence Fe$^{3+}$. Using first-principles techniques, we developed a three-orbital tight-binding model that reproduces the {\it ab initio} band structure near the Fermi level. Including Hubbard and Hund couplings and studying the model via the density matrix renormalization group and Lanczos methods, we constructed the ground state phase diagram. A robust region where the block state $\uparrow \uparrow \downarrow \downarrow \uparrow \uparrow \downarrow \downarrow$ is stabilized was unveiled. The analog state in iron ladders, employing 2$\times$2 ferromagnetic blocks, is by now well-established, but in chains a block magnetic order has not been observed yet in real materials. The phase diagram also contains a large region of canonical staggered spin order $\uparrow \downarrow \uparrow \downarrow \uparrow \downarrow \uparrow$ at very large Hubbard repulsion. At the block to staggered transition region, a novel phase is stabilized with a mixture of both states: an inhomogeneous orbital-selective charge density wave with the exotic spin configuration $\uparrow \uparrow \downarrow \uparrow \downarrow \downarrow \uparrow \downarrow$. Our predictions for Na$_2$FeSe$_2$ may guide crystal growers and neutron scattering experimentalists towards the realization of block states in one-dimensional iron-selenide chain materials.