Many processes in chemistry, such as those of photochemical, magnetic, or spintronic interest, require a comprehensive treatment of spin and spin couplings. These are treated naturally with relativistic Hamiltonians, but combining DFT with multicomponent relativistic methods such as X2C also requires a general non-collinear framework for evaluation of common exchange-correlation functionals. The ability to treat local magnetization density is key to understanding the time-dependent properties and dynamics of localized spin centers in ground and excited states. A non-collinear formulation of time-dependent Kohn-Sham DFT allows for a nonzero local torque, although still satisfying the zero torque theorem with no global torque. This has been able to describe the spectroscopic properties of both closed and open shell systems, such as L-edge X-ray absorption. Although the use of relativistic DFT has been successful in describing small systems with transition metals or heavy atoms, the much higher cost of 2- or 4-component methods still limits its potential applications for studying larger molecules or nanostructures. The use of density functional embedding theory can enable the treatment of much larger systems with relativistic methods by performing high level calculations only on a subsystem.  Additionally, the study of excited states in a strong electromagnetic field, or with multiple pulses for multidimensional spectroscopy is possible using real-time time-dependent theories.<br/>

Recent advances in relativistic TDDFT

256th National Meeting (2018)

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