Origin of doping-induced suppression and reemergence of magnetism in LaFeAsO$_{1-x}$H$_x$

TL;DR

This study uses advanced theoretical methods to explain the complex magnetic behavior in hydrogen-doped LaFeAsO, revealing how doping influences electron correlations and orbital contributions, and clarifying experimental observations of magnetic phases.

Contribution

It provides a detailed theoretical explanation for the doping-dependent magnetic phases and orbital effects in LaFeAsO$_{1-x}$H$_x$, integrating electron occupation, structural changes, and correlation effects.

Findings

Magnetic moment exhibits a minimum at intermediate doping levels.

Two separate antiferromagnetic phases are explained by opposing effects of doping.

Orbital polarization shifts from $d_{xz/yz}$ to $d_{xy}$ with doping.

Abstract

We investigate the evolution of magnetic properties as a function of hydrogen doping in iron based superconductor LaFeAsO$_{1-x}$H$_x$ using the dynamical mean-field theory combined with the density-functional theory. We find that two independent consequences of the doping, the increase of the electron occupation and the structural modification, have the opposite effects on the strength of electron correlation and magnetism, resulting in the minimum of the calculated magnetic moment around the intermediate doping level as a function of $x$. Our result provides a natural explanation for the puzzling recent experimental discovery of the two separated antiferromagnetic phases at low and high doping limits. Furthermore, the increase of orbital occupation and correlation strength with the doping results in reduced orbital polarization of $d_{xz/yz}$ orbitals and the enhanced role of $d_{xy}$ orbital in the magnetism at high doping levels, and their possible implications to the superconductivity are discussed in line with the essential role of the magnetism.