Problems with reconciling density functional theory calculations with experiment in ferropnictides

TLDR

First‑principles calculations of magnetic and electronic properties of LaFeAsO‑based superconductors show substantial controversy, with differing quantitative values and divergent interpretations of magnetic interactions. The study systematically compares four first‑principles methods to determine whether fully converged full‑potential all‑electron calculations agree, thereby advancing understanding of the magnetic interactions. Four first‑principles methods are employed, revealing that the itinerant magnetic ground state, soft moments, and long‑range reciprocal‑space interactions drive the sensitivity of the results.

Abstract

First-principles calculations of magnetic and, to a lesser extent, electronic properties of the LaFeAsO-based superconductors show substantial apparent controversy, as opposed to most weakly or strongly correlated materials. Not only do different reports disagree about quantitative values but there is also a schism in terms of interpreting the basic physics of the magnetic interactions in this system. In this paper, we present a systematic analysis using four different first-principles methods and show that while there is an unusual sensitivity to computational details, well-converged full-potential all-electron results are fully consistent among themselves. What makes results so sensitive and the system so different from simple local magnetic moments interacting via basic superexchange mechanisms is the itinerant character of the calculated magnetic ground state, where very soft magnetic moments and long-range interactions are characterized by a particular structure in the reciprocal (as opposed to real) space. Therefore, unravelling the magnetic interactions in their full richness remains a challenging but utterly important task.