Empirical Magnetic Structure of Frustrated Spin Systems

TL;DR

This paper demonstrates that powder neutron scattering data can be used to determine the magnetic structures of frustrated spin systems, enabling detailed characterization without single-crystal samples through ab initio reverse Monte Carlo refinement.

Contribution

It introduces a novel methodology using reverse Monte Carlo refinement to solve magnetic structures of frustrated systems from powder data, overcoming traditional limitations.

Findings

Successfully determined magnetic structures of spin ices, spin liquids, and molecular magnets.

Revealed detailed spin correlation functions and scattering patterns.

Validated approach as a powerful tool for studying exotic magnetic states.

Abstract

Frustrated magnetism plays a central role in the phenomenology of exotic quantum states. However, because the magnetic structures of frustrated systems are aperiodic, there has always been the problem that they cannot be determined using traditional crystallographic techniques. Here we show that the magnetic component of powder neutron scattering data is actually sufficiently information-rich to drive magnetic structure solution for frustrated systems, including spin ices, spin liquids, and molecular magnets. Consequently, single-crystal samples are not prerequisite for detailed characterisation of exotic magnetic states. Our methodology employs ab initio reverse Monte Carlo refinement, making informed use of an additional constraint that minimises variance in local spin environments. By refining atomistic spin configurations, we obtain at once (i) a magnetic structure "solution" - i.e. the orientation of classical spin vectors - (ii) the spin correlation functions, and (iii) the full three-dimensional magnetic scattering pattern.