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[2+2] Photocycloaddition Reaction Dynamics of Triplet Pyrimidines
Yang, Chunfan; Yu, Youqing; Liu, Kunhui; Song, Di; Wu, Lidan; Su, Hongmei
刊名JOURNAL OF PHYSICAL CHEMISTRY A
2011-06-02
DOI10.1021/jp201418r
115期:21页:5335-5345
收录类别SCI
文章类型Article
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]FLUORESCENCE UP-CONVERSION ; EXCITED-STATE DYNAMICS ; ULTRAFAST INTERNAL-CONVERSION ; ELECTRONIC GROUND-STATE ; SINGLE-STRANDED-DNA ; THYMINE DIMERIZATION ; AQUEOUS-SOLUTION ; CONICAL INTERSECTIONS ; NUCLEIC-ACIDS ; URACIL
英文摘要Taking the 266 nm excited pyrimidine (uracil or thymine) with cyclopentene as model reaction systems, we have examined the photoproduct formation dynamics from the [2 + 2] photocycloaddition reactions of triplet pyrimidines in solution and provided mechanistic insights into this important DNA photodamage reaction. By combining two compliment methods of nanosecond time-resolved transient IR and UV-vis laser flash-photolysis spectroscopy, the photoproduct formation dynamics as well as the triplet quenching kinetics are measured. Characteristic IR absorption bands due to photoproduct formation have been observed and product quantum yields are determined to be similar to 0.91% for uracil and similar to 0.41% for thymine. Compared to the measured large quenching rate constants of triplet uracil (1.5 x 10(9) M(-1)s(-1)) or thymine (0.6 x 10(9) M(-1)s(-1)) by cyclopentene, the inefficiency in formation of photoproducts indicates competitive physical quenching processes may exist on the route leading to photoproducts, resulting in very small product yields eventually. Such an energy wasting process is found to be resulted from T(1)/S(0) surface crossings by the hybrid density functional calculations, which compliments the experiments and reveals the reaction mechanism.
语种英语
WOS记录号WOS:000290914500012
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/142282
专题中国科学院大连化学物理研究所
作者单位Chinese Acad Sci, Inst Chem, State Key Lab Mol React Dynam, Beijing Natl Lab Mol Sci BNLMS, Beijing 100190, Peoples R China
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Yang, Chunfan,Yu, Youqing,Liu, Kunhui,et al. [2+2] Photocycloaddition Reaction Dynamics of Triplet Pyrimidines[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2011,115(21):5335-5345.
APA Yang, Chunfan,Yu, Youqing,Liu, Kunhui,Song, Di,Wu, Lidan,&Su, Hongmei.(2011).[2+2] Photocycloaddition Reaction Dynamics of Triplet Pyrimidines.JOURNAL OF PHYSICAL CHEMISTRY A,115(21),5335-5345.
MLA Yang, Chunfan,et al."[2+2] Photocycloaddition Reaction Dynamics of Triplet Pyrimidines".JOURNAL OF PHYSICAL CHEMISTRY A 115.21(2011):5335-5345.
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