Dynamical transition orbitals: A particle–hole description in real-time TDDFT dynamics

نویسندگان

چکیده

We expand the concept of natural transition orbitals in context real-time time-dependent density functional theory (RT-TDDFT) and show its application practical calculations. Kohn–Sham single-particle wavefunctions are propagated RT-TDDFT simulation, physical properties remain invariant under their unitary transformation. In this work, we exploit gauge freedom orbitals, which is widely used linear-response TDDFT, for obtaining a particle–hole description simulation. While TDDFT to study electronic excitation, can be employed more generally simulate non-equilibrium electron dynamics. Studying dynamics terms dynamic transitions pairs is, however, not straightforward By constructing through projecting wave functions onto occupied/unoccupied eigenstate subspaces, that linear combinations pair resulting hole/particle form new gauge, refer as dynamical orbitals. demonstrate utility framework analyze simulations optical excitation stopping description.

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ژورنال

عنوان ژورنال: Journal of Chemical Physics

سال: 2021

ISSN: ['1520-9032', '1089-7690', '0021-9606']

DOI: https://doi.org/10.1063/5.0035435