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Cu$_4$ triplet clusters form the relevant spin entity for the formation oflong-range magnetic order in the cluster magnet Cu$_2$OSeO$_3$. Usingtime-resolved Raman spectroscopy, we probed photoinduced spin and latticedynamics in this Mott insulator. Multiple ps-decade spin-lattice relaxationdynamics is observed, evidencing a separation of the order parameter dynamicsinto disordering of long-range and internal spin cluster order. Our studyexemplifies the double order parameter dynamics of generalized molecularcrystals of charge, spin, and orbital nature.

Coupled dynamics of long-range and internal spin cluster order in Cu$_{2}$OSeO$_{3}$