Zhao, D.; He, X.; Ayers, P.W.; Liu, S. Excited-State Polarizabilities: A Combined Density Functional Theory and Information-Theoretic Approach Study. Molecules2023, 28, 2576.
Zhao, D.; He, X.; Ayers, P.W.; Liu, S. Excited-State Polarizabilities: A Combined Density Functional Theory and Information-Theoretic Approach Study. Molecules 2023, 28, 2576.
Zhao, D.; He, X.; Ayers, P.W.; Liu, S. Excited-State Polarizabilities: A Combined Density Functional Theory and Information-Theoretic Approach Study. Molecules2023, 28, 2576.
Zhao, D.; He, X.; Ayers, P.W.; Liu, S. Excited-State Polarizabilities: A Combined Density Functional Theory and Information-Theoretic Approach Study. Molecules 2023, 28, 2576.
Abstract
Accurate and efficient determination of excited-state polarizabilities (α) is an open problem both experimentally and computationally. Following our previous work, [Phys. Chem. Chem. Phys. 2023, 25, 2131−2141], where one can employ simple ground-state density-based functions from the information-theoretic approach (ITA) to accurately and efficiently predict the macromolecular polarizabilities, we aim to predict the lowest excited-state polarizabilities in this work. The philosophy is to use density-based functions to depict the excited-state polarizabilities. As a proof-of-principle application, employing 2-(2′-hydroxyphenyl)benzimidazole and its derivatives as model systems, we have verified that either with the ground-state (S0) or excited-state (S1) densities as input, ITA quantities can be strongly correlated with the excited-state polarizabilities. When the transition densities are considered, both S0 and S1 polarizabilities are in good relationships with some ITA quantities. Furthermore, excitation and emission energies can be predicted based on multivariant linear regression equations of ITA quantities.
Keywords
density functional theory; information theory; excited-state polarizability; ESIPT (excited-state intramolecular proton transfer)
Subject
CHEMISTRY, Physical Chemistry
Copyright:
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