DICP OpenIR
Excited state non-adiabatic dynamics of pyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study
Wu, Guorong1,2,3; Neville, Simon P.4; Schalk, Oliver1,5; Sekikawa, Taro1,6; Ashfold, Michael N. R.7; Worth, Graham A.4; Stolow, Albert1,8,9
Source PublicationJOURNAL OF CHEMICAL PHYSICS
2015-02-21
DOI10.1063/1.4907529
Volume142Issue:7
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectPhysics, Atomic, Molecular & Chemical
WOS Research AreaPhysics
WOS KeywordNEAR-ULTRAVIOLET PHOTOLYSIS ; CONICAL INTERSECTIONS ; PHOTODISSOCIATION DYNAMICS ; EXCITATION-SPECTRA ; ELECTRONIC STATES ; DEPENDENT HARTREE ; ATOM ELIMINATION ; WAVE-PACKET ; MOLECULES ; FURAN
AbstractThe dynamics of pyrrole excited at wavelengths in the range 242-217 nm are studied using a combination of time-resolved photoelectron spectroscopy and wavepacket propagations performed using the multi-configurational time-dependent Hartree method. Excitation close to the origin of pyrrole's electronic spectrum, at 242 and 236 nm, is found to result in an ultrafast decay of the system from the ionization window on a single timescale of less than 20 fs. This behaviour is explained fully by assuming the system to be excited to the A(2)(pi sigma*) state, in accord with previous experimental and theoretical studies. Excitation at shorter wavelengths has previously been assumed to result predominantly in population of the bright A(1)(pi pi*) and B-2(pi pi*) states. We here present time-resolved photoelectron spectra at a pump wavelength of 217 nm alongside detailed quantum dynamics calculations that, together with a recent reinterpretation of pyrrole's electronic spectrum [S. P. Neville and G. A. Worth, J. Chem. Phys. 140, 034317 (2014)], suggest that population of the B-1(pi sigma*) state (hitherto assumed to be optically dark) may occur directly when pyrrole is excited at energies in the near UV part of its electronic spectrum. The B-1(pi sigma*) state is found to decay on a timescale of less than 20 fs by both N-H dissociation and internal conversion to the A(2)(pi sigma*) state. (C) 2015 AIP Publishing LLC.
Language英语
WOS IDWOS:000350547500015
Citation statistics
Cited Times:39[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/146064
Collection中国科学院大连化学物理研究所
Affiliation1.Natl Res Council Canada, Ottawa, ON K1A 0R6, Canada
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, 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 Birmingham, Sch Chem, Birmingham B15 2TT, W Midlands, England
5.Stockholm Univ, AlbaNova Univ Ctr, Dept Phys, S-10961 Stockholm, Sweden
6.Hokkaido Univ, Dept Appl Phys, Kita Ku, Sapporo, Hokkaido 0608628, Japan
7.Univ Bristol, Sch Chem, Bristol BS8 1TS, Avon, England
8.Univ Ottawa, Dept Chem, Ottawa, ON K1N 6N5, Canada
9.Univ Ottawa, Dept Phys, 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 pyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study[J]. JOURNAL OF CHEMICAL PHYSICS,2015,142(7).
APA Wu, Guorong.,Neville, Simon P..,Schalk, Oliver.,Sekikawa, Taro.,Ashfold, Michael N. R..,...&Stolow, Albert.(2015).Excited state non-adiabatic dynamics of pyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study.JOURNAL OF CHEMICAL PHYSICS,142(7).
MLA Wu, Guorong,et al."Excited state non-adiabatic dynamics of pyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study".JOURNAL OF CHEMICAL PHYSICS 142.7(2015).
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