DICP OpenIR
Excited state non-adiabatic dynamics of N-methylpyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study
Wu, Guorong1,2,3; Neville, Simon P.4; Schalk, Oliver1,5; Sekikawa, Taro6; Ashfold, Michael N. R.7; Worth, Graham A.8; Stolow, Albert1,4,9
Source PublicationJOURNAL OF CHEMICAL PHYSICS
2016-01-07
ISSN0021-9606
DOI10.1063/1.4938423
Volume144Issue:1
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS Research AreaChemistry ; Physics
WOS KeywordNEAR-ULTRAVIOLET PHOTOLYSIS ; PHOTODISSOCIATION DYNAMICS ; UV PHOTODISSOCIATION ; ELECTRONIC STATES ; ATOM ELIMINATION ; PYRROLE ; MOLECULES ; PHOTOCHEMISTRY ; APPROXIMATION ; IONIZATION
AbstractThe dynamics of N-methylpyrrole following excitation at wavelengths in the range 241.5-217.0 nm were studied using a combination of time-resolved photoelectron spectroscopy (TRPES), ab initio quantum dynamics calculations using the multi-layer multi-configurational time-dependent Hartree method, as well as high-level photoionization cross section calculations. Excitation at 241.5 and 236.2 nm results in population of the A(2)(pi sigma*) state, in agreement with previous studies. Excitation at 217.0 nm prepares the previously neglected B-1(pi 3p(y)) Rydberg state, followed by prompt internal conversion to the A(2)(pi sigma*) state. In contrast with the photoinduced dynamics of pyrrole, the lifetime of the wavepacket in the A(2)(pi sigma*) state was found to vary with excitation wavelength, decreasing by one order of magnitude upon tuning from 241.5 nm to 236.2 nm and by more than three orders of magnitude when excited at 217.0 nm. The order of magnitude difference in lifetimes measured at the longer excitation wavelengths is attributed to vibrational excitation in the A(2)(pi sigma*) state, facilitating wavepacket motion around the potential barrier in the N-CH3 dissociation coordinate. (C) 2016 AIP Publishing LLC.
Language英语
WOS IDWOS:000368617300015
PublisherAMER INST PHYSICS
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/171437
Collection中国科学院大连化学物理研究所
Corresponding AuthorStolow, Albert
Affiliation1.Natl Res Council Canada, 100 Sussex Dr, Ottawa, ON K1A 0R6, Canada
2.Chinese Acad Sci, State Key Lab Mol React Dynam, Dalian Inst Chem Phys, Dalian 116023, Liaoning, Peoples R China
3.Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China
4.Univ Ottawa, Dept Chem, 10 Marie Curie, Ottawa, ON K1N 6N5, Canada
5.Stockholm Univ, Dept Phys, AlbaNova Univ Ctr, Roslagstullsbacken 21, S-10691 Stockholm, Sweden
6.Hokkaido Univ, Dept Appl Phys, Kita Ku, Kita 13 Nishi 8, Sapporo, Hokkaido 0608628, Japan
7.Univ Bristol, Sch Chem, Bristol BS8 1TS, Avon, England
8.Univ Birmingham, Sch Chem, Birmingham B15 2TT, W Midlands, England
9.Univ Ottawa, Dept Phys, 150 Louis Pasteur, Ottawa, ON K1N 6N5, Canada
Recommended Citation
GB/T 7714
Wu, Guorong,Neville, Simon P.,Schalk, Oliver,et al. Excited state non-adiabatic dynamics of N-methylpyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study[J]. JOURNAL OF CHEMICAL PHYSICS,2016,144(1).
APA Wu, Guorong.,Neville, Simon P..,Schalk, Oliver.,Sekikawa, Taro.,Ashfold, Michael N. R..,...&Stolow, Albert.(2016).Excited state non-adiabatic dynamics of N-methylpyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study.JOURNAL OF CHEMICAL PHYSICS,144(1).
MLA Wu, Guorong,et al."Excited state non-adiabatic dynamics of N-methylpyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study".JOURNAL OF CHEMICAL PHYSICS 144.1(2016).
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