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Photoreaction channels of the guanine-cytosine base pair explored by long-range corrected TDDFT calculations
| Title: | Photoreaction channels of the guanine-cytosine base pair explored by long-range corrected TDDFT calculations |
| Authors: | Yamazaki, Shohei Browse this author | | Taketsugu, Tetsuya Browse this author →KAKEN DB |
| Issue Date: | 17-Apr-2012 |
| Publisher: | Royal Society of Chemistry |
| Journal Title: | Physical Chemistry Chemical Physics |
| Volume: | 14 |
| Issue: | 25 |
| Start Page: | 8866 |
| End Page: | 8877 |
| Publisher DOI: | 10.1039/c2cp23867e |
| PMID: | 22596076 |
| Abstract: | Photoinduced processes in the Watson-Crick guanine-cytosine base pair are comprehensively studied by means of long-range corrected (LC) TDDFT calculations of potential energy profiles using the LC-BLYP and CAM-B3LYP functionals. The ab initio CC2 method and the conventional TDDFT method with the B3LYP functional are also employed to assess the reliability of the LC-TDDFT method. The present approach allows us to compare the potential energy profiles at the same computational level for excited-state reactions of the base pair, including single and double proton transfer between the bases and nonradiative decay via ring puckering in each base. In particular, long-range correction to the TDDFT method is critical for a qualitatively correct description of the proton transfer reactions. The calculated energy profiles exhibit low barriers for out-of-plane deformation of the guanine moiety in the locally-excited state, which is expected to lead to a conical intersection with the ground state, as well as for single proton transfer from guanine to cytosine with the well-known electron-driven proton transfer mechanism. Thus the present results suggest that both processes can compete in hydrogen-bonded base pairs and play a significant role in the mechanism of photostability. |
| Rights: | Phys. Chem. Chem. Phys., 2012,14, 8866-8877 - Reproduced by permission of the PCCP Owner Societies |
| Type: | article (author version) |
| URI: | http://hdl.handle.net/2115/53176 |
| Appears in Collections: | 理学院・理学研究院 (Graduate School of Science / Faculty of Science) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)
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Submitter: 山崎 祥平
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