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Perspectives on double-excitations in TDDFT |
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| Authors: | Peter Elliott Sharma GoldsonChris Canahui Neepa T Maitra |
| Institution: | Department of Physics and Astronomy, Hunter College and the City University of New York, 695 Park Avenue, New York 10065, USA |
| Abstract: | 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. |
| Keywords: | TDDFT DFT Kohn-Sham Double excitations Linear-response Quadratic response Second-order response Autoionization Semiclassical Frozen Gaussian Density matrix Density functional Adiabatic approximation |
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