Nonadiabatic decay dynamics of 9H-guanine in aqueous solution
文献类型：期刊论文
| 作者 | Heggen, Berit2; Lan, Zhenggang1; Thiel, Walter2 |
| 刊名 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS
 |
| 出版日期 | 2012 |
| 卷号 | 14期号:22页码:8137-8146 |
| 英文摘要 | The nonadiabatic decay of the biologically relevant guanine tautomer (9H-guanine) in aqueous solution has been investigated by trajectory surface hopping simulations in a quantum mechanical-molecular mechanical (QM-MM) framework. The QM part (9H-guanine) was treated at the semiempirical OM2/MRCI level, while the MM part (water) was described by the TIP3P force field. The optimized geometries for the relevant minima and conical intersections are qualitatively similar for 9H-guanine in the gas phase and in aqueous solution, while there are notable solvent-induced shifts in the computed vertical excitation energies (up to about 0.4 eV). Overall, the results from the static OM2/MRCI-based calculations are in reasonable agreement with the available ab initio and experimental data. The dynamics simulations show ultrafast nonradiative decay for 9H-guanine in water that is even slightly faster than in the gas phase, with time constants of 20 fs and around 0.3 ps for the S-2 -> S-1 and S-1 -> S-0 internal conversions, respectively. They predict a change in the S-1 -> S-0 decay mechanism when going from the gas phase to aqueous solution: the major pathway for 9H-guanine in water involves a conical intersection with an out-of-plane distortion of the carbonyl oxygen atom, which does not play any significant role in the gas phase, where the decay mainly proceeds via two other conical intersections characterized by ring distortions and out-of-plane displacement of the amino group, respectively. Possible reasons for this change in the mechanism are analyzed. |
| WOS标题词 | Science & Technology ; Physical Sciences |
| 类目[WOS] | Chemistry, Physical ; Physics, Atomic, Molecular & Chemical |
| 研究领域[WOS] | Chemistry ; Physics |
| 关键词[WOS] | EXCITED-STATE DYNAMICS ; NUCLEIC-ACID BASES ; ULTRAFAST INTERNAL-CONVERSION ; MOLECULAR-DYNAMICS ; GAS-PHASE ; NONRADIATIVE DECAY ; RNA BASES ; SEMIEMPIRICAL METHODS ; ELECTRONIC-SPECTRA ; GUANINE TAUTOMERS |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000304102200030 |
| 公开日期 | 2015-12-24 |
| 源URL | [http://ir.qibebt.ac.cn/handle/337004/6389]  |
| 专题 | 青岛生物能源与过程研究所_仿真模拟团队 |
| 作者单位 | 1.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China 2.Max Planck Inst Kohlenforsch, D-45470 Mulheim, Germany |
| 推荐引用方式 GB/T 7714 | Heggen, Berit,Lan, Zhenggang,Thiel, Walter. Nonadiabatic decay dynamics of 9H-guanine in aqueous solution[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2012,14(22):8137-8146. |
| APA | Heggen, Berit,Lan, Zhenggang,&Thiel, Walter.(2012).Nonadiabatic decay dynamics of 9H-guanine in aqueous solution.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,14(22),8137-8146. |
| MLA | Heggen, Berit,et al."Nonadiabatic decay dynamics of 9H-guanine in aqueous solution".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 14.22(2012):8137-8146. |
入库方式： OAI收割
来源：青岛生物能源与过程研究所
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