Ultrafast Spin Dynamics and Photoinduced Insulator-to-Metal Transition in α-RuCl(3)

[Image: see text] Laser-induced ultrafast demagnetization is a phenomenon of utmost interest and attracts significant attention because it enables potential applications in ultrafast optoelectronics and spintronics. As a spin–orbit coupling assisted magnetic insulator, α-RuCl(3) provides an attractive platform to explore the physics of electronic correlations and unconventional magnetism. Using time-dependent density functional theory, we explore the ultrafast laser-induced dynamics of the electronic and magnetic structures in α-RuCl(3). Our study unveils that laser pulses can introduce ultrafast demagnetizations, accompanied by an out-of-equilibrium insulator-to-metal transition in a few tens of femtoseconds. The spin response significantly depends on the laser wavelength and polarization on account of the electron correlations, band renormalizations, and charge redistributions. These findings provide physical insights into the coupling between the electronic and magnetic degrees of freedom in α-RuCl(3) and shed light on suppressing the long-range magnetic orders and reaching a proximate spin liquid phase for two-dimensional magnets on an ultrafast time scale.