Abstract

Cu$_4$ triplet clusters form the relevant spin entity for the formation of long-range magnetic order in the cluster magnet Cu$_2$OSeO$_3$. Using time-resolved Raman spectroscopy, we probed photoinduced spin and lattice dynamics in this Mott insulator. Multiple ps-decade spin-lattice relaxation dynamics is observed, evidencing a separation of the order parameter dynamics into disordering of long-range and internal spin cluster order. Our study exemplifies the double order parameter dynamics of generalized molecular crystals of charge, spin, and orbital nature.

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