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题名: Nonadiabatic dissociation dynamics in H2O: Competition between rotationally and nonrotationally mediated pathways
作者: Yuan, Kaijun1;  Cheng, Yuan1;  Cheng, Lina1;  Guo, Qing1;  Dai, Dongxu1;  Wang, Xiuyan1;  Yang, Xueming1;  Dixon, Richard N.2
关键词: photochemistry ;  water ;  photodissociation ;  stereodynamics ;  VUV photolysis
刊名: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
发表日期: 2008-12-09
DOI: 10.1073/pnas.0807719105
卷: 105, 期:49, 页:19148-19153
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology
类目[WOS]: Multidisciplinary Sciences
研究领域[WOS]: Science & Technology - Other Topics
英文摘要: The photochemistry of H2O in the VUV region is important in interstellar chemistry. Whereas previous studies of the photodissociation used excitation via unbound states, we have used a tunable VUV photolysis source to excite individual levels of the rotationally structured (C) over tilde state near 124 nm. The ensuing OH product state distributions were recorded by using the H-atom Rydberg tagging technique. Experimental results indicate a dramatic variation in the OH product state distributions and its stereodynamics for different resonant states. Photodissociation of H2O((C) over tilde) in rotational states with k(a)' = 0 occurs exclusively through a newly discovered homogeneous coupling to the (A) over tilde state, leading to OH products that are vibrationally hot (up to v = 13), but rotationally cold. In contrast, for H2O in rotationally excited states with k(a)' > 0, an additional pathway opens through Coriolis-type coupling to the (B) over tilde state surface. This yields extremely rotationally hot and vibrationally cold ground state OH(X) and electronically excited OH(A) products, through 2 different mechanisms. In the case of excitation via the 1(10) <- 0(00) transition the H atoms for these 2 product channels are ejected in completely different directions. Quantum dynamical models for the (C) over tilde -state photodissociation clearly support this remarkable dynamical picture, providing a uniquely detailed illustration of nonadiabatic dynamics involving at least 4 electronic surfaces.
关键词[WOS]: MULTIPHOTON IONIZATION SPECTROSCOPY ;  OH PROMPT EMISSION ;  PHOTODISSOCIATION DYNAMICS ;  MOLECULAR PREDISSOCIATION ;  2 COMETS ;  WATER ;  NM ;  STATES ;  JET ;  D2O
语种: 英语
WOS记录号: WOS:000261706600025
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/141116
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
2.Univ Bristol, Sch Chem, Bristol BS8 1TS, Avon, England

Recommended Citation:
Yuan, Kaijun,Cheng, Yuan,Cheng, Lina,et al. Nonadiabatic dissociation dynamics in H2O: Competition between rotationally and nonrotationally mediated pathways[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2008,105(49):19148-19153.
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