Sulfur Oxidation State and Substituents Influenced Multifunctional Organic Luminophores in BTP Core for OLEDs: A Computational Study on RTP, TADF Emitter and Sensitizer

J Phys Chem A. 2023 Dec 21;127(50):10570-10582. doi: 10.1021/acs.jpca.3c05259. Epub 2023 Dec 8.

Abstract

The exploration of triplet excitons in thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) molecules has become a subject of significant attention and interest in recent studies. This study employed density functional theory (DFT) and time-dependent DFT theoretical methods to delve into the intricate relationship between the molecular structure and properties of molecules designed with the oxidation of sulfur atoms (S, SO, and SO2) in benzothiazinophenothiazine (BTP) core units. The calculations revealed that as the oxidation state of the sulfur atom increased, the BTP derivatives exhibited elevated ionization potentials (IPs), electron affinities (EAs), and triplet energies (ET), accompanied by reduced reorganization energies (λ), singlet energies (ES), and a S1-T1 energy gap (ΔEST). Additionally, the decrease in the exchange energy prompts a shift in the excited-state properties of molecules, transitioning them from hybridized local and charge transfer (HLCT) to charge transfer (CT) in the S1 state while maintaining their HLCT character in the T1 state. The sulfur oxidation process systematically decreases spin-orbit coupling magnitudes in the S1-T1 and T1-S0 pathways while increasing the KRISC rate, signifying a reduced propensity for phosphorescence radiative decay in oxidized molecules. Thorough investigations have explored the screening effect and orbital mixing of lone pair electrons in sulfur atoms, satisfying the desired criteria for a multifunctional RTP, TADF emitter and sensitizer.