Simulation of Low-Lying Singlet and Triplet Excited States of Multiple-Resonance-Type Thermally Activated Delayed Fluorescence Emitters by Delta Self-Consistent Field (ΔSCF) Method

J Phys Chem A. 2021 Dec 9;125(48):10373-10378. doi: 10.1021/acs.jpca.1c08900. Epub 2021 Dec 1.

Abstract

The delta self-consistent field (ΔSCF) method was applied to the simulation of low-lying singlet and triplet excited states of multiple-resonance (MR)-type thermally activated delayed fluorescence (TADF) molecules, which form a promising group for organic light-emitting diode (OLED) emitters. A comparison with the experimental values of 13 emitters from the literature showed that ΔSCF gave fairly accurate S1 and T1 excitation energies (mean absolute errors (MAEs) of 0.092 and 0.055 eV, respectively) as well as quite accurate ΔEST (S1-T1 gap, MAE of 0.041 eV), which could not be calculated with sufficient accuracy by the conventional time-dependent density functional theory (TDDFT). ΔSCF also demonstrated its utility for the analysis of photophysical properties through a simulation of the reverse intersystem crossing (RISC) process of an MR-type emitter.