Comparative Study of TDDFT and TDDFT-based STEOM-DLPNO-CCSD Calculations for Predicting the Excited-state Properties of MR-TADF

Overview

Journal Heliyon

Specialty Social Sciences

Date 2024 May 23

PMID 38779014

Authors

Sunwoo Kang

Taekyung Kim

Affiliations

Soon will be listed here.

Abstract

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.

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