ABSTRACT
We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate α-RuCl3 to investigate the nonequilibrium dynamics of its antiferromagnetically ordered zigzag groundstate after photoexcitation. A systematic study of the transient magnetic linear dichroism under different experimental conditions (temperature, external magnetic field, photoexcitation density) gives direct access to the dynamical interplay of charge excitations with the zigzag ordered state on ultrashort time scales. We observe a rather slow initial demagnetization (few to 10s of ps) followed by a long-lived non-thermal antiferromagnetic spin-disordered state (100-1000s of ps), which can be understood in terms of holons and doublons disordering the antiferromagnetic background after photoexcitation. Varying temperature and fluence in the presence of an external magnetic field reveals two distinct photoinduced dynamics associated with the zigzag and quantum paramagnetic disordered phases. The photo-induced non-thermal spin-disordered state shows universal compressed-exponential recovery dynamics related to the growth and propagation of zigzag domains on nanosecond time scales, which is interpreted within the framework of the Fatuzzo-Labrune model for magnetization reversal. The study of nonequilibrium states in strongly correlated materials is a relatively unexplored topic, but our results are expected to be extendable to a large class of Mott-Hubbard insulator materials with strong spin-orbit coupling.
ABSTRACT
We use circular dichroism (CD) in time- and angle-resolved photoemission spectroscopy (trARPES) to measure the femtosecond charge dynamics in the topological insulator (TI) [Formula: see text]. We detect clear CD signatures from topological surface states (TSS) and surface resonance (SR) states. In time-resolved measurements, independently from the pump polarization or intensity, the CD shows a dynamics which provides access to the unexplored electronic evolution in unoccupied states of [Formula: see text]. In particular, we are able to disentangle the unpolarized electron dynamics in the bulk states from the spin-textured TSS and SR states on the femtosecond timescale. Our study demonstrates that photoexcitation mainly involves the bulk states and is followed by sub-picosecond transport to the surface. This provides essential details on intra- and interband scattering in the relaxation process of TSS and SR states. Our results reveal the significant role of SRs in the subtle ultrafast interaction between bulk and surface states of TIs.
