1B2(1Σu+) excited state decay dynamics in CS2

被引:30
作者
Townsend, Dave [1 ]
Satzger, Helmut
Ejdrup, Tine
Lee, Anthony M. D.
Stapelfeldt, Henrik
Stolow, Albert
机构
[1] Natl Res Council Canada, Steacie Inst Mol Sci, Ottawa, ON K1A 0R6, Canada
[2] Univ Aarhus, Dept Chem, DK-8000 Aarhus C, Denmark
[3] Queens Univ, Dept Chem, Kingston, ON K7L 3N6, Canada
[4] Queens Univ, Dept Phys, Kingston, ON K7L 3N6, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
D O I
10.1063/1.2403137
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The authors report time resolved photoelectron spectra of the B-1(2)((1)Sigma(+)(u)) state of CS2 at pump wavelengths in the region of 200 nm. In contrast to previous studies, the authors find that the predissociation dynamics is not well described by a single exponential decay. Biexponential modeling of the authors' data reveals a rapid decay pathway (tau < 50 fs), in addition to a longer lived channel (tau similar to 350-650 fs) that displays a marked change in apparent lifetime when the polarization of the pump laser is rotated with respect to that of the probe. Since the initially populated B-1(2)((1)Sigma(+)(u)) state may decay to form either S(D-1) or S(P-3) products (the latter produced via a spin-orbit induced crossing from a singlet to a triplet electronic surface), this lifetime observation may be rationalized in terms of changes in the relative ionization cross section of these singlet and triplet states of CS2 as a function of laser polarization geometry. The experimentally observed lifetime of the longer lived channel is therefore a superposition of these two pathways, both of which decay on very similar time scales. (c) 2006 American Institute of Physics.
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页数:10
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