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Finite-temperature-based time-dependent density-functional theory method for static electron correlation systems
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DOI：10.1063/1.5144527.png)
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Abstract
En 中文
In this study, we developed a time-dependent density-functional theory (TDDFT) with a finite-temperature (FT) scheme, denoted as FT-TDDFT. We introduced the concept of fractional occupation numbers for random phase approximation equation and evaluated the excited-state electronic entropy terms with excited-state occupation number. The orbital occupation numbers for the excited state were evaluated from the change in the ground-state electron configuration with excitation and deexcitation coefficients. Furthermore, we extended the FT formulation to the time-dependent density-functional tight-binding (TDDFTB) method for larger systems, denoted as FT-TDDFTB. Numerical assessment for the FT-(TD)DFT method showed smooth potential curves for double-bond rotation of ethylene in both ground and excited states. Excited-state calculations based on the FT-TDDFTB method were applied to the uniform pi -stacking columns composed of trioxotriangulene, possessing neutral radicals in strong correlation systems.
Keywords:
2ND-ORDER PERTURBATION-THEORY
COUPLED-CLUSTER METHOD
EXCITATION-ENERGIES
TIGHT-BINDING
OCCUPATION NUMBERS
RESPONSE THEORY
IMPLEMENTATION
ATOMS
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