Ab initio insight into ultrafast nonadiabatic decay of hypoxanthine: keto-N7H and keto-N9H tautomers
文献类型：期刊论文
| 作者 | Guo, Xugeng1,2; Lan, Zhenggang3; Cao, Zexing1,2 |
| 刊名 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS
 |
| 出版日期 | 2013 |
| 卷号 | 15期号:26页码:10777-10782 |
| 中文摘要 | Nonadiabatic dynamics simulations at the SA-CASSCF level were performed for the two most stable keto-N7H and keto-N9H tautomers of hypoxanthine in order to obtain deep insight into the lifetime of the optically bright S1(1pp*) excited state and the relevant decay mechanisms. Supporting calculations on the ground-state (S0) equilibrium structures and minima on the crossing seams of both tautomers were carried out at the MR-CIS and CASSCF levels. These studies indicate that there are four slightly different kinds of conical intersections in each tautomer, exhibiting a chiral character, each of which dominates a barrierless reaction pathway. Moreover, both tautomers reveal the ultrafast S1 - S0 decay, in which the S1 state of keto-N9H in the gas phase has a lifetime of 85.5 fs, whereas that of keto-N7H has a longer lifetime of 137.7 fs. An excellent agreement is found between the present results and the experimental value of 130 _ 20 fs in aqueous solution (Chen and Kohler, Phys. Chem. Chem. Phys., 2012, 14, 10677–10689). |
| 英文摘要 | Nonadiabatic dynamics simulations at the SA-CASSCF level were performed for the two most stable keto-N7H and keto-N9H tautomers of hypoxanthine in order to obtain deep insight into the lifetime of the optically bright S-1((1)pi pi*) excited state and the relevant decay mechanisms. Supporting calculations on the ground-state (S-0) equilibrium structures and minima on the crossing seams of both tautomers were carried out at the MR-CIS and CASSCF levels. These studies indicate that there are four slightly different kinds of conical intersections in each tautomer, exhibiting a chiral character, each of which dominates a barrierless reaction pathway. Moreover, both tautomers reveal the ultrafast S-1 -> S-0 decay, in which the S1 state of keto-N9H in the gas phase has a lifetime of 85.5 fs, whereas that of keto-N7H has a longer lifetime of 137.7 fs. An excellent agreement is found between the present results and the experimental value of 130 +/- 20 fs in aqueous solution. |
| WOS标题词 | Science & Technology ; Physical Sciences |
| 学科主题 | 仿真与模拟 |
| 类目[WOS] | Chemistry, Physical ; Physics, Atomic, Molecular & Chemical |
| 研究领域[WOS] | Chemistry ; Physics |
| 关键词[WOS] | 2ND-ORDER PERTURBATION-THEORY ; MR-CI LEVEL ; EXCITED-STATES ; ANALYTIC EVALUATION ; MOLECULAR-DYNAMICS ; NONRADIATIVE DECAY ; AQUEOUS-SOLUTION ; PROTON-TRANSFER ; COUPLING TERMS ; PROGRAM |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000320321600024 |
| 公开日期 | 2014-03-21 |
| 源URL | [http://ir.qibebt.ac.cn:8080/handle/337004/1626]  |
| 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.Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China 2.Xiamen Univ, Coll Chem & Chem Engn, Fujian Prov Key Lab Theoret & Computat Chem, Xiamen 361005, Peoples R China 3.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao Key Lab Solar Energy Utilizat & Energy St, Qingdao 266101, Peoples R China |
| 推荐引用方式 GB/T 7714 | Guo, Xugeng,Lan, Zhenggang,Cao, Zexing. Ab initio insight into ultrafast nonadiabatic decay of hypoxanthine: keto-N7H and keto-N9H tautomers[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2013,15(26):10777-10782. |
| APA | Guo, Xugeng,Lan, Zhenggang,&Cao, Zexing.(2013).Ab initio insight into ultrafast nonadiabatic decay of hypoxanthine: keto-N7H and keto-N9H tautomers.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,15(26),10777-10782. |
| MLA | Guo, Xugeng,et al."Ab initio insight into ultrafast nonadiabatic decay of hypoxanthine: keto-N7H and keto-N9H tautomers".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 15.26(2013):10777-10782. |
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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