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arxiv 1101.3379 v1 pith:CPQNSLOZ submitted 2011-01-18 physics.chem-ph cond-mat.mtrl-scicond-mat.other

Perspectives on double-excitations in TDDFT

classification physics.chem-ph cond-mat.mtrl-scicond-mat.other
keywords double-excitationstddftdoubleexcitationadiabaticappearingapproachapproximation
verification ladder T0 review T1 audit T2 compute T3 formal T4 reserved
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The adiabatic approximation in time-dependent density functional theory (TDDFT) yields reliable excitation spectra with great efficiency in many cases, but fundamentally fails for states of double excitation character. We discuss how double-excitations are at the root of some of the most challenging problems for TDDFT today. We then present new results for (i) the calculation of autoionizing resonances in the helium atom, (ii) understanding the nature of the double excitations appearing in the quadratic response function, and (iii) retrieving double-excitations through a real-time semiclassical approach to correlation in a model quantum dot.

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