Recent advances in ultrafast spectroscopy have allowed for the study of electron dynamics at the sub-femtosecond time scale. These experimental advances introduce the need for explicitly time-dependent theoretical methods that can accurately model the quantum processes on the ultrafast time scale. In addition, theoretical methods are needed that can model spin transitions in these processes through the inclusion of relativistic effects. The time-dependent spin-orbit configuration interaction (TDSOCI) method is an <i>ab initio</i> method for accurately modeling the relativistic electron dynamics of transition metal compounds and other small molecules as they interact with ultrashort laser pulses. The addition of spin-orbit coupling to TDCI allows for the study of spin flip dynamics in an extendable theoretical framework. Here, the TDSOCI methodology is extended to include dissipative effects from the interaction of the system and its environment. Through a propagation of the reduced density matrix, the effects of energy and phase dissipation can be included, and these methods are applied to study the spin dynamics of Fe-containing compounds.

Relativistic electron dynamics via time-dependent spin-orbit configuration interaction theory

ACS Spring Meeting 2021

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