Hydroxyl super rotors from vacuum ultraviolet photodissociation of water

被引：44

作者：

Chang, Yao ^{[1
,2
]}

Yu, Yong ^{[1
,3
]}

Wang, Heilong ^{[1
,4
]}

Hu, Xixi ^{[5
]}

Li, Qinming ^{[1
,3
]}

Yang, Jiayue ^{[1
]}

Su, Shu ^{[1
]}

He, Zhigang ^{[1
]}

Chen, Zhichao ^{[1
]}

Che, Li ^{[4
]}

Wang, Xingan ^{[2
]}

Zhang, Weiqing ^{[1
]}

Wu, Guorong ^{[1
]}

Xie, Daiqian ^{[5
]}

Ashfold, Michael N. R. ^{[6
]}

Yuan, Kaijun ^{[1
]}

Yang, Xueming ^{[1
,7
]}

机构：

[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, 457 Zhongshan Rd, Dalian 116023, Peoples R China

[2] Univ Sci & Technol China, Sch Chem & Mat Sci, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China

[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

[4] Dalian Maritime Univ, Sch Sci, Dept Phys, 1 Linghai Rd, Dalian 116026, Liaoning, Peoples R China

[5] Nanjing Univ, Sch Chem & Chem Engn, Inst Theoret & Computat Chem, Key Lab Mesoscop Chem, Nanjing 210093, Jiangsu, Peoples R China

[6] Univ Bristol, Sch Chem, Bristol BS8 1TS, Avon, England

[7] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1期

基金：

中国国家自然科学基金; 英国工程与自然科学研究理事会;

关键词：

DISSOCIATION DYNAMICS; 121.6; NM; H2O; MOLECULE; BOND; D2O; PHOTOCHEMISTRY; SPECTROSCOPY; COMPETITION; SPECTRA;

D O I：

10.1038/s41467-019-09176-z

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Hydroxyl radicals (OH) play a central role in the interstellar medium. Here, we observe highly rotationally excited OH radicals with energies above the bond dissociation energy, termed OH "super rotors", from the vacuum ultraviolet photodissociation of water. The most highly excited OH(X) super rotors identified at 115.2 nm photolysis have an internal energy of 4.86 eV. A striking enhancement in the yield of vibrationally-excited OH super rotors is detected when exciting the bending vibration of the water molecule. Theoretical analysis shows that bending excitation enhances the probability of non-adiabatic coupling between the (B) over tilde and (X) over tilde states of water at collinear O-H-H geometries following fast internal conversion from the initially excited (D) over tilde state. The present study illustrates a route to produce extremely rotationally excited OH(X) radicals from vacuum ultraviolet water photolysis, which may be related to the production of the highly rotationally excited OH(X) radicals observed in the interstellar medium.

引用

页数：7

共 41 条

[31] SELECTIVELY BREAKING THE O-H BOND IN HOD [J].

VANDERWAL, RL ;

SCOTT, JL ;

CRIM, FF .

JOURNAL OF CHEMICAL PHYSICS, 1990, 92 (01) :803-805

[32] FLUCTUATIONS IN ABSORPTION-SPECTRA AND FINAL PRODUCT STATE DISTRIBUTIONS FOLLOWING PHOTODISSOCIATION PROCESSES [J].

VONDIRKE, M ;

HEUMANN, B ;

KUHL, K ;

SCHRODER, T ;

SCHINKE, R .

JOURNAL OF CHEMICAL PHYSICS, 1994, 101 (03) :2051-2068

[33] Photodissociation dynamics of H2O at 111.5 nm by a vacuum ultraviolet free electron laser [J].

Wang, Heilong ;

Yu, Yong ;

Chang, Yao ;

Su, Shu ;

Yu, Shengrui ;

Li, Qinming ;

Tao, Kai ;

Ding, Hongli ;

Yang, Jaiyue ;

Wang, Guanglei ;

Che, Li ;

He, Zhigang ;

Chen, Zhichao ;

Wang, Xingan ;

Zhang, Weiqing ;

Dai, Dongxu ;

Wu, Guorong ;

Yuan, Kaijun ;

Yang, Xueming .

JOURNAL OF CHEMICAL PHYSICS, 2018, 148 (12)

[34] Dissociation dynamics of the water molecule on the (A)over-tilde 1B1 electronic surface [J].

Yang, XF ;

Hwang, DW ;

Lin, JJ ;

Ying, X .

JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (23) :10597-10604

[35] High-gain harmonic-generation free-electron laser [J].

Yu, LH ;

Babzien, M ;

Ben-Zvi, I ;

DiMauro, LF ;

Doyuran, A ;

Graves, W ;

Johnson, E ;

Krinsky, S ;

Malone, R ;

Pogorelsky, I ;

Skaritka, J ;

Rakowsky, G ;

Solomon, L ;

Wang, XJ ;

Woodle, M ;

Yakimenko, V ;

Biedron, SG ;

Galayda, JN ;

Gluskin, E ;

Jagger, J ;

Sajaev, V ;

Vasserman, I .

SCIENCE, 2000, 289 (5481) :932-934

[36] Photochemistry of the Water Molecule: Adiabatic versus Nonadiabatic Dynamics [J].

Yuan, Kaijun ;

Dixon, Richard N. ;

Yang, Xueming .

ACCOUNTS OF CHEMICAL RESEARCH, 2011, 44 (05) :369-378

[37] Tunable VUV photochemistry using Rydberg H-atom time-of-flight spectroscopy [J].

Yuan, Kaijun ;

Cheng, Lina ;

Cheng, Yuan ;

Guo, Qing ;

Dai, Dongxu ;

Yang, Xueming .

REVIEW OF SCIENTIFIC INSTRUMENTS, 2008, 79 (12)

[38] Nonadiabatic dissociation dynamics in H2O: Competition between rotationally and nonrotationally mediated pathways [J].

Yuan, Kaijun ;

Cheng, Yuan ;

Cheng, Lina ;

Guo, Qing ;

Dai, Dongxu ;

Wang, Xiuyan ;

Yang, Xueming ;

Dixon, Richard N. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (49) :19148-19153

[39] Signatures of non-adiabatic dynamics in the fine-structure state distributions of the OH((X)over-tilde/(A)over-tilde) products in the B-band photodissociation of H2O [J].

Zhou, Linsen ;

Xie, Daiqian ;

Guo, Hua .

JOURNAL OF CHEMICAL PHYSICS, 2015, 142 (12)

[40] State to state photodissociation dynamics of D2O in the B band [J].

Zhou, Linsen ;

Lin, Guang-Shuang-Mu ;

Xie, Daiqian .

JOURNAL OF CHEMICAL PHYSICS, 2013, 139 (11)

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