Near and Above Ionization Electronic Excitations with Non-Hermitian Real-Time Time-Dependent Density Functional Theory.
作者： Kenneth Lopata , Niranjan Govind
DOI: 10.1021/CT400569S
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摘要: We present a real-time time-dependent density functional theory (RT-TDDFT) prescription for capturing near and post-ionization excitations based on non-Hermitian von Neumann matrix propagation with atom-centered basis sets, tuned range-separated DFT, phenomenological imaginary molecular orbital-based absorbing potential to mimic coupling the continuum. The computed extreme ultraviolet absorption spectra acetylene (C2H2), water (H2O), Freon 12 (CF2Cl2) agree well electron energy loss spectroscopy (EELS) data over range of 0-50 eV. removes spurious high-energy finite artifacts, yielding correct bound-to-bound transitions, metastable (autoionizing) resonance states, consistent overall shapes.
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