Assessing the atomic moment picture of spin dynamics: the perspective of ab initio magnon wavefunction

Our understanding of collective spin fluctuation in materials relies largely on Heisenberg-type spin Hamiltonians. Implicit in these spin models is the atomic moment picture that in transverse spin dynamics the magnetization around an atom undergoes precessional motion as a rigid moment, which has been challenged by emerging theoretical and experimental advances.To assess the validity of the atomic moment picture in spin dynamics, however, necessitates magnon wavefunctions from ab initio methods without a priori spin models.To this end, we develop an efficient model-free ab initio method for computing magnon spectrum and wavefunctions. Niu-Kleinman's adiabatic spin-wave dynamics is reformulated using linear perturbation theory into a generalized eigenvalue problem, which can be solved to produce magnon spectrum and wavefunctions without assuming atomic moments. We have implemented this method in the framework of density functional perturbation theory (DFPT). A dynamical extension of Niu-Kleinman equation of motion is proposed to improve inaccurate predicted magnon energies due to imperfect adiabaticity at higher energies. Based on so-obtained ab initio magnon wavefunctions, we find the atomic moment picture to be valid in typical ferromagnets and antiferromagnets, but fails in the molecular orbital crystal Na_2IrO_3. Our results suggest that the usual spin Hamiltonian approach should be taken with a grain of salt, and possible experimental ramification on the issue is discussed.