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Exact time-dependent density functional theory for non-perturbative dynamics of helium atom

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arxiv 2105.08656 v2 pith:UB2PYMB2 submitted 2021-05-18 physics.chem-ph

classification physics.chem-ph
keywords exactkohn-shamatomdynamicsheliumtime-dependentadiabaticapproximate
verification ladder T0 review T1 audit T2 compute T3 formal
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By inverting the time-dependent Kohn-Sham equation for a numerically exact dynamics of the helium atom, we show that the dynamical step and peak features of the exact correlation potential found previously in one-dimensional models persist for real three-dimensional systems. We demonstrate that the Kohn-Sham and true current-densities differ by a rotational component. The results have direct implications for approximate TDDFT calculations of atoms and molecules in strong fields, emphasizing the need to go beyond the adiabatic approximation, and highlighting caution in quantitative use of the Kohn-Sham current.

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