Kang Sunwoo, Kim Taekyung
Department of Chemistry, Dankook University, Cheonan, Chungnam, 31116, South Korea.
Department of Materials Science and Engineering, Hongik University, Sejongsi, 30016, South Korea.
Heliyon. 2024 May 11;10(10):e30926. doi: 10.1016/j.heliyon.2024.e30926. eCollection 2024 May 30.
The time dependent density functional theory (TDDFT) and TDDFT/similarity transformed EOM domain-based local pair natural orbital CCSD (STEOM-DLPNO-CCSD) calculations were explored to estimate their validity in predicting the excited-state properties of multi-resonant thermally activated delayed fluorescence (MR-TADF) materials. Obviously, it was demonstrated that TDDFT calculation is inadequate to provide the quantitative prediction of the lowest singlet excited-state (S), the lowest triplet excited-state (T), and ΔE. On the other hand, TDDFT/STEOM-DNLPNO-CCSD calculation reveals the superior prediction of S, T, and ΔE that are in quantitative agreement with experiments. More importantly, it was found that TD-LC-HPBE/STEOM-DLPNO-CCSD calculation provides the most accurate prediction of S, T, and ΔE. Accordingly, we suggest that TD-LC-HPBE/STEOM-DLPNO-CCSD calculation should be utilized to compute the excited-states properties of MR-TADF materials accurately.
探索了含时密度泛函理论（TDDFT）以及TDDFT/相似变换的基于能域的局域对自然轨道耦合簇单双激发（STEOM-DLPNO-CCSD）计算，以评估它们在预测多共振热激活延迟荧光（MR-TADF）材料激发态性质方面的有效性。显然，结果表明TDDFT计算不足以对最低单重激发态（S）、最低三重激发态（T）以及ΔE进行定量预测。另一方面，TDDFT/STEOM-DNLPNO-CCSD计算显示出对S、T和ΔE的卓越预测，与实验结果在定量上相符。更重要的是，发现TD-LC-HPBE/STEOM-DLPNO-CCSD计算对S、T和ΔE提供了最准确的预测。因此，我们建议应采用TD-LC-HPBE/STEOM-DLPNO-CCSD计算来准确计算MR-TADF材料的激发态性质。
