Single-Laser-Pulse-Driven Thermal Limit of the Quasi-Two-Dimensional Magnetic Ordering in Sr_{2}IrO_{4}

Abstract

Upon femtosecond-laser stimulation, generally materials are expected to recover back to their thermal-equilibrium conditions, with only a few exceptions reported. Here, we demonstrate that deviation from the thermal-equilibrium pathway can be induced in canonical 3D antiferromagnetically (AFM) ordered Sr_{2}IrO_{4} by a single 100-fs-laser pulse, appearing as losing long-range magnetic correlation along one direction into a glassy condition. We further discover a “critical-threshold ordering” behavior for fluence above approximately 12 mJ/cm^{2}, which we show corresponds to the smallest thermodynamically stable c-axis correlation length needed to maintain long-range quasi-two-dimensional AFM order. We suggest that this behavior arises from the crystalline anisotropy of the magnetic-exchange parameters in Sr_{2}IrO_{4}, whose strengths are associated with distinctly different timescales. As a result, they play out very differently in the ultrafast recovery processes, compared with the thermal-equilibrium evolution. Thus, our observations are expected to be relevant to a wide range of problems in the nonequilibrium behavior of low-dimensional magnets and other related ordering phenomena.