Theoretical simulations on the excited state dynamics of thymine agree on the involvement of two excited states relevant for the internal conversion back to the S 0 state; (τ 1 = 60 ± 30 fs) and photoelectron experiments 116 (τ 1 =37 fs), while the latter slow timescale has been experimentally well documented. Therefore, the excited state PESs as well as the NAMD results by BH&HLYP functionals can serve as a reference. A detailed description of NAMD simulations performed in the current study is presented in Section IV of Supporting Information. It was shown that the PESs around the conical intersection between S 1 and S 2 (CI 21 ) along the bond-alternation coordinate (BLA) critically affects the NAMD simulations. The same S 1 and S 2 surfaces along the BLA of thymine were calculated by DTCAM-VEE as well as DTCAM-AEE and the results are presented in Fig. . The S 1 by DTCAM-VEE is about 0.54 eV lower than that of BH&HLYP at FC, while it is about 1.0 eV lower near S 1,min . On the other hand, the reduction of S 2 surface is relatively constant along the entire PES. The significantly stabilized S 1 after the conical intersection is clearly seen in the squared difference plots (squared red line) of Fig. . Consequently, the selectively stabilized S 1,min by DTCAM-VEE accelerates the internal conversion S 1 → S 0 in our NAMD simulations as shown in Fig. , where S 0 population (dotted line) increases rapidly as compared to that of BH&HLYP, producing half of S 0 populations in about 100 fs.