We have developed a method of quantitatively predicting radiative and nonradiative decay rate constants. The method is based on the excited-state computation and rate-constant calculation with the Fermi golden rule. First, we briefly review the rate constant formulae. Second, we present the application of our method to the excited-state decay mechanism of photoexcited benzophenone. We successfully reproduce all the experimentally obtained rate constants, including those for fluorescence, phosphorescence, and intersystem crossing. Calculated results show that the dominant decay channel is the indirect S1→T2→T1 process. Finally, we highlight the application to multiple-resonance thermally activated delayed fluorescence (MR-TADF) mechanism of DABNA-1. We successfully reproduce experimental photophysical properties, including electronic-transition rate constants, lifetimes, and PLQYs relevant to TADF. We show that TADF in DABNA-1 occurs via a higher triplet state (T2).
View full abstract