Cu4 triplet clusters form the relevant spin entity for the formation of long-range magnetic order in the cluster magnet Cu2OSeO3. 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.
@article{arxiv.1902.05329,
title = {Coupled dynamics of long-range and internal spin cluster order in Cu$_{2}$OSeO$_{3}$},
author = {R. B. Versteeg and J. Zhu and C. Boguschewski and F. Sekiguchi and A. Sahasrabudhe and K. Budzinauskas and P. Padmanabhan and P. Becker and D. I. Khomskii and P. H. M. van Loosdrecht},
journal= {arXiv preprint arXiv:1902.05329},
year = {2019}
}