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Ultrafast Excited-State Dynamics of 6-Azauracil Studied by Femtosecond Transient Absorption Spectroscopy
Hua, XinZhong; Hua, LinQiang; Liu, XiaoJun
2015-12-31
Source PublicationJOURNAL OF PHYSICAL CHEMISTRY A
Volume119Issue:52Pages:12985-12989
SubtypeArticle
AbstractThe excited-state dynamics of 6-azauracil in different solvents have been studied using femtosecond transient absorption spectroscopy. The molecule is populated to the S-2 state with a pump pulse at 264 nm. Broad-band white light continuum which covers from 320 to 600 nm is used as the probe. With a global fitting analysis of the measured transient spectra, three decay time constants, i.e., <0.3, 5.2 +/- 0.1, and >1000 ps, are directly obtained in the solvent of acetonitrile. These newly observed lifetime constants are important in clarifying its decay dynamics as well as in providing a criterion for the ultrafast dynamics simulations in 6-azauracil using quantum chemical theories. In combination with previous theoretical works, the main decay channel is proposed: the initially populated S-2 decays to S-1 through internal conversion in <0.3 ps, followed by an intersystem crossing from S-1 to T-1 in 5.2 +/- 0.1 ps. The >1000 ps component is due to the decay of the T-1 state. A comparison of the excited-state dynamics in different solvents reveals that the decay from S, to T-1 shows a clear dependence on the polarity of the solvents. With higher polarity, the S-1 excited state decays faster. This observation is in line with the prediction by Etinski et al. [Phys. Chem. Chem. Phys. 2010, 12, 15665-15671], where a blue-shift of the T-1 state potential energy surface leading to an increase of the intersystem crossing rate was proposed. With the new information obtained in the present measurement, a clearer picture of the decay dynamics of 6-azauracil on the S-2 excited state is provided.
WOS HeadingsScience & Technology ; Physical Sciences
DOI10.1021/acs.jpca.5b08975
WOS KeywordFLUORESCENCE UP-CONVERSION ; ELECTRONIC GROUND-STATE ; RELAXATION MECHANISMS ; URACIL DERIVATIVES ; AQUEOUS-SOLUTION ; THYMINE ; ACETONITRILE ; PATHWAYS ; DECAY ; BASES
Indexed BySCI
Language英语
WOS Research AreaChemistry ; Physics
WOS SubjectChemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS IDWOS:000367705400009
Citation statistics
Cited Times:7[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.apm.ac.cn/handle/112942/9144
Collection原子分子光物理研究部
AffiliationChinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Peoples R China
Recommended Citation
GB/T 7714
Hua, XinZhong,Hua, LinQiang,Liu, XiaoJun. Ultrafast Excited-State Dynamics of 6-Azauracil Studied by Femtosecond Transient Absorption Spectroscopy[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2015,119(52):12985-12989.
APA Hua, XinZhong,Hua, LinQiang,&Liu, XiaoJun.(2015).Ultrafast Excited-State Dynamics of 6-Azauracil Studied by Femtosecond Transient Absorption Spectroscopy.JOURNAL OF PHYSICAL CHEMISTRY A,119(52),12985-12989.
MLA Hua, XinZhong,et al."Ultrafast Excited-State Dynamics of 6-Azauracil Studied by Femtosecond Transient Absorption Spectroscopy".JOURNAL OF PHYSICAL CHEMISTRY A 119.52(2015):12985-12989.
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