Spin-orbit coupling (SOC), which can induce spin flip during the relaxation of photoexcited charge carrier, plays a crucial role in spin dynamics. In this work, we have used time-domain ab initio nonadiabatic molecular dynamics (NAMD) method to study the SOC induced ultrafast demagnetization in Ni at $300\mathrm{K}$. The spin-diabatic representation using spin-polarized Kohn-Sham (KS) basis sets and spin-adiabatic representation using spinor basis sets have been applied, and both of them achieve demagnetization in Ni with a timescale around $100\mathrm{fs}$. The spin-diabatic representation suggests a picture that the electron-phonon coupling (EPC) provides direct energy relaxation channel among the same-spin states, while the SOC can induce spin flip. After photoexcitation, it is found the spin-minority electrons relax to the same-spin states rather than the opposite-spin states, since EPC is larger than SOC by one order of magnitude. By contrast, for the spin-majority electrons, spin flip occurs since there are no empty same-spin states as electron acceptor above the Fermi level. The different relaxation pathways for spin-majority and spin-minority electrons induce the demagnetization. The spin-adiabatic representation provides an Elliott-Yafet spin-phonon scattering picture. The SOC induced reduction of magnetic moment in Ni may induce magnon to drive further demagnetization. The ab initio NAMD simulation provides a critical angle to understand how the SOC and EPC affect demagnetization process in Ni.

• Received 26 October 2021
• Revised 23 January 2022
• Accepted 28 January 2022

DOI:https://doi.org/10.1103/PhysRevB.105.085142