<br/>The time-dependent Hartree-Fock (TDHF) and time-dependent density functional theory (TDDFT) equations are widely used as a first approximation to understanding electronic excited states. While the natural transition orbital method has allowed transitions to be viewed in a traditional orbital picture, the extension to multicomponent molecular orbitals such as those used in generalized Hartree-Fock (GHF) or generalized Kohn-Sham (GKS) is less straightforward due to mixing of spin-components and the inherent inclusion of spin- flip transitions in TDGHF/TDGKS. An extension of natural transition orbitals to the two- component framework is presented, in addition to a discussion of the practical aspects of visualizing two-component orbitals. Unlike the single-component analog, the method explicitly describes the spin and frequently obtains solutions with multiple orbitals such as an equal mixture of α and β components in a singlet transition. The method is presented using calculations of a small model cluster of a ZnO semiconducting quantum dot as a motivating example. Comparison with other techniques based on visualizing the density or density difference show that the approaches yield similar, though sometimes complimentary information.

Natural transition orbitals for complex 2-component TDDFT

2019 Fall National Meeting

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