Electronic structure theory can accurately compute numerical solutions of the time-independent Schrödinger equation for ground-state molecules in the Born-Oppenheimer approximation. However, the cost of such calculations is often impractical (e.g., full configuration interaction) such that more approximate methods are used. Kohn-Sham density functional theory (KS-DFT) has established itself as a pragmatic choice for electronic structure applications due to the good accuracy-to-cost ratio for modern approximate density functionals. However, the transition from non-relativistic to relativistic KS-DFT introduces additional cost that may become prohibitive as the size and number of atoms increases. Thus, it is desirable to treat a subsystem relativistically while treating everything else with non-relativistic KS-DFT. We are developing quantum embedding where a subsystem is treated with relativistic 2-component KS-DFT, and the rest is treated with unrestricted KS-DFT. We will discuss the handling of the resulting magnetic field from open-shell fragments and show application to transition-metal defects in ZnO quantum dots.

Embedding relativistic 2-component Kohn-Sham density functional theory in a non-relativistic quantum environment

2019 Fall National Meeting

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