English

Charge Transfer with a Spin. I: A Generalized CASSCF Framework for Investigating Charge Transfer in the Presence of Spin-Orbit Coupling

Chemical Physics 2026-02-13 v2

Abstract

We present a generalized extension of the recently developed electron/hole-transfer Dynamically-weighted State-Averaged Constrained CASSCF (eDSC/hDSC) method to model charge transfer in the presence of spin-orbit coupling (SOC) for systems containing an odd number of electrons. Our approach incorporates complex-valued spinor orbitals and incorporates four electronic configurations in describing ground-excited state curve crossings between Kramers-restricted doublet states. The method achieves smooth potential energy surfaces and rapid self-consistent field (SCF) convergence across a wide range of spin-orbit coupling strengths, providing an efficient framework for investigating charge transfer processes in the presence of nontrivial spin degrees of freedom.

Keywords

Cite

@article{arxiv.2602.07746,
  title  = {Charge Transfer with a Spin. I: A Generalized CASSCF Framework for Investigating Charge Transfer in the Presence of Spin-Orbit Coupling},
  author = {Alok Kumar and Zhen Tao and Joseph E. Subotnik and Tian Qiu},
  journal= {arXiv preprint arXiv:2602.07746},
  year   = {2026}
}