Inelastic light scattering in the spin cluster Mott insulator Cu${}_2$OSeO${}_3$

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.

arXiv comment10 pages, 6 figures

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Cited by in corpus (3)

• Experimental signatures of quantum and topological states in frustrated magnetism
• Raman spectroscopy of alpha-FeOOH (goethite) near antiferromagnetic to paramagnetic phase transition
• Site-specific electronic and magnetic excitations of the skyrmion material Cu${}_2$OSeO${}_3$