Ultrafast signatures of spin and orbital order in antiferromagnetic α-Sr2CrO4

Abstract We used femtosecond optical spectroscopy to study ultrafast spin and orbital ordering dynamics in the antiferromagnetic Mott insulator α-Sr2CrO4. This chromate system possesses multiple spin and orbital ordered phases, and therefore could enable us to study the unique interplay between these collective phases through their non-equilibrium response to photoexcitation. Here, by varying the pump photon energy, we selectively drove inter-site spin hopping between neighboring Cr t2g orbitals and charge transfer-type transitions between oxygen 2p and Cr eg orbitals. The resulting transient reflectivity dynamics revealed temperature-dependent anomalies across the Neel temperature for spin ordering as well as the transition temperatures linked to different types of orbital order. Our results reveal distinct relaxation timescales for spin and orbital orders in α-Sr2CrO4 and provide experimental evidence for the phase transition at TO, possibly related to antiferro-type orbital ordering.