Excited-State Polarizabilities: A Combined Density Functional Theory and Information-Theoretic Approach Study

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 (S0) density-related functions from the information-theoretic approach (ITA) to accu-rately and efficiently evaluate the macromolecular polarizabilities, we aim to predict the lowest excited-state (S1) polarizabilities in this work. The philosophy is to use density-based functions to depict the excited-state polarizabilities. As a proof-of-principle appli-cation, employing 2-(2′-hydroxyphenyl)benzimidazole and its substituents as model sys-tems, we have verified that either with S0 or 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 mul-tivariant linear regression equations of ITA quantities.