In this work, we present a framework of ab initio time-dependent variational approach to effectively explore the spin phase space in the presence of a homogenous magnetic field. Complex generalized Hartree-Fock and density function theory in the spinor formalism is implemented with London orbitals. A Pauli matrix representation of the C-GHF is introduced to separate spin contributions from scalar part of the Fock matrix. The spin phase transition in the molecular system in the presence of a strong magnetic field is investigated. Non-collinear spin configurations are observed during the phase transition from singlet to triplet state. The competing driving forces of exchange coupling and spin Zeeman effect have been shown to govern the spin phase transition and transition rate. The energetic contributions of the spin Zeeman, orbital Zeeman, and diamagnetic terms to the potential energy surface are also analyzed.

Modeling spin-dynamics with relativistic two-component time-dependent electronic structure method

2019 Spring National Meeting

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