Time-Dependent Relativistic Electron Dynamics of Laser-Driven Transition Metal Complexes

Advances in ultrafast spectroscopy have increased the viability of simulating and predicting electron dynamics in molecular systems, such as electronic density and spin behaviors through the use of specifically controlled external perturbations such as laser pulses. The use and development of time-dependent methodologies for modelling the dynamics of electronic systems computationally is an active field and has potential application for the research and development of molecular systems that utilize relativistic spin properties, such as dye-sensitized solar cells and molecular switches.



One approach to simulating the electron dynamics of molecular systems is with time-dependent spin-orbit configuration interaction (TD-SOCI), a method which propagates a relativistic configuration interaction wavefunction with external perturbations. The underlying theory of TD-SOCI will be covered, and progress on the use of TD-SOCI for the analysis and modelling transition metal complexes interacting with applied laser pulses will be highlighted. Induced metal-to-ligand charge transfers and spin-flips can be demonstrated and visualized by one-body operators applied to the TD-SOCI wavefunction, such as electronic density, spin density, and electronic current density.