Modeling Magneto‐Photoabsorption Using Time‐Dependent Complex Generalized Hartree‐Fock
Abstract Magneto‐optical spectroscopy provides a glimpse into the hidden electronic structure of molecules and materials that normally cannot be resolved with regular optical absorption spectroscopy. The magneto‐optical signal is difficult to simulate computationally due to the necessity of modeling perturbations from both uniform magnetic and oscillating electric fields. In this work, we introduce a time‐dependent complex generalized Hartree‐Fock framework for calculating electronic magneto‐optical spectra of atomic and molecular systems. Complex‐valued gauge including atomic orbitals are used in a non‐perturbative treatment of the uniform magnetic field. The magneto‐photoabsorption spectra of atomic alkalis and aromatic systems are investigated with a focus on understanding how spectroscopic signals change in the presence of a uniform magnetic field.