Inelastic Light Scattering In The Spin Cluster Mott Insulator Cu2oseo3

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 Cu2OSeO3 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 Cu2OSeO3 can be regarded as a solid-state molecular crystal of spin nature.