Non-collinear magnetism engendered by a hidden another order

TL;DR

This paper demonstrates that in PrO$_2$, high-rank multipolar interactions, rather than traditional Heisenberg exchange, drive the non-collinear magnetic order, revealing a hidden multipolar origin of magnetism.

Contribution

It shows that high-rank multipolar interactions are the primary cause of magnetic order in PrO$_2$, challenging the standard Heisenberg-based paradigm.

Findings

Non-collinear 2k magnetic structure in PrO$_2$ is due to high-rank multipolar interactions.

Heisenberg interactions are negligible in explaining PrO$_2$ magnetic order.

The model accounts for experimental observations like exchange splitting and magnetic field evolution.

Abstract

Standard microscopic approach to magnetic orders is based on assuming a Heisenberg form for inter-atomic exchange interactions. These interactions are considered as a driving force for the ordering transition with magnetic moments serving as the primary order parameter. Any higher-rank multipoles appearing simultaneously with such magnetic order are typically treated as auxiliary order parameters rather than a principal cause of the transition. In this study, we show that these traditional assumptions are violated in the case of PrO$_2$. Evaluating the full set of Pr-Pr superexchange interactions from a first-principles many-body technique we find that its unusual non-collinear 2k magnetic structure stems from high-rank multipolar interactions, and that the corresponding contribution of the Heisenberg interactions is negligible. The observed magnetic order in PrO$_2$ is thus auxiliary to high-rank "hidden" multipoles. Within this picture we consistently account for previously unexplained experimental observations like the magnitude of exchange splitting and the evolution of magnetic structure in external field. Our findings challenge the standard paradigm of observable magnetic moments being the driving force for magnetic transitions.