Inelastic light scattering in the spin cluster Mott insulator Cu$_{2}$OSeO$_{3}$

TL;DR

This study investigates high-energy spin excitations in the spin cluster Mott insulator Cu$_{2}$OSeO$_{3}$ using Raman scattering, revealing multiple optical magnon modes and strong magnetoelectric coupling, supporting its analogy to a molecular crystal of spins.

Contribution

It provides the first detailed observation of high-energy spin cluster excitations and their coupling to phonons in Cu$_{2}$OSeO$_{3}$, highlighting its molecular crystal-like spin structure.

Findings

Multiple high-energy optical magnon modes observed

Raman activity due to Elliot-Loudon scattering mechanism

Strong temperature dependence indicating magnetoelectric coupling

Abstract

Clusters of single spins form the relevant spin entities in the formation of long-range magnetic order in spin cluster Mott insulators. Such type of spin order bears resemblance to molecular crystals, and we therefore may expect a prototypical spin wave spectrum which can be divided into low-energy external and high-energy internal cluster spin wave modes. Here, we study high-energy spin cluster excitations in the spin cluster Mott insulator Cu$_{2}$OSeO$_{3}$ by means of spontaneous Raman scattering. Multiple high-energy optical magnon modes are observed, of which the Raman-activity is shown to originate in the Elliot-Loudon scattering mechanism. Upon crossing the long-range ordering transition temperature the magnetic modes significantly broaden, corresponding to scattering from localized spin excitations within the spin clusters. Different optical phonon modes show a strong temperature dependence, evidencing a strong magnetoelectric coupling between optical phonons and the high-energy spin cluster excitations. Our results support the picture that Cu$_{2}$OSeO$_{3}$ can be regarded as a solid-state molecular crystal of spin nature.