Time-resolved photoelectron angular distributions as a means of studying polyatomic nonadiabatic dynamics

Journal of Chemical Physics

Volumn 113, Issue 5, 2000, Pages 1677-1680

  Seideman, Tamar ^a  

^a NATIONAL RESEARCH COUNCIL CANADA   (Canada)

Author keywords

[No Author keywords available]

Indexed keywords

APPROXIMATION THEORY; ELECTRON ENERGY LEVELS; IONIZATION; LIGHT POLARIZATION; MOLECULAR DYNAMICS; MOLECULAR STRUCTURE; NUMERICAL METHODS; POLYOLEFINS; SPECTROSCOPIC ANALYSIS;

EIGHT CARBON MEMBER OCTATETRANE; IONIZED ORBITAL; LINEAR POLYENES; NONRADIATIVE TRANSITIONS; POLYATOMIC NONADIABATIC DYNAMICS; TIME RESOLVED PHOTOELECTRON ANGULAR DISTRIBUTIONS;

ELECTRON TRANSITIONS;

EID: 0034250774     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.481968     Document Type: Article

References (33)

1. Several recent reviews and many references are collected in Faraday Discuss. Chem. Soc. 2000, 115.
2. Several of the historical reviews about nonradiative transitions are given in (a) J. Jortner, S. A. Rice, and R. M. Hochstrasser, Adv. Photochem. 7, 149 (1969);
3. (b) B. R. Henry and W. Siebrand, in Molecular Luminescence, edited by E. C. Lim (Benjamin, New York, 1969), p. 423. See also E. C. Lim, p. 469 in the same volume;
4. (b) B. R. Henry and W. Siebrand, in Molecular Luminescence, edited by E. C. Lim (Benjamin, New York, 1969), p. 423. See also E. C. Lim, p. 469 in the same volume;
5. (c) M. A. El-Sayed, in Ref. 1 (b), p. 715,
6. (d) K. F. Freed, in Radiationless Processes in Molecules and Condensed Phases, edited by F. K. Fong (Springer, Berlin, 1976), p. 23.
7. (a) G. Stock, R. Schneider, and W. Domcke, J. Chem. Phys. 90, 7184 (1989).;
8. (b) M. Seel and W. Domcke, ibid. 95, 7806 (1991).
9. B. Kim, C. P. Schick, and P. M. Weber, J. Chem. Phys. 103, 6903 (1995).
10. The effect of different configurations of the dark and ion states on the PED is illustrated by D. R. Cyr and C. C. Hayden, J. Chem. Phys. 10, 771 (1996).
11. W. Radloff et al. Chem. Phys. Lett. 281, 20 (1997).
12. V. Blanchet, M. Zgierski, T. Seideman, and A. Stolow, Nature (London) 401, 52 (1999).
13. V. Blanchet et al., Faraday Discuss. Chem. Soc. (in press).
14. L. Wang, H. Kohguchi, and T. Suzuki, Faraday Discuss. Chem. Soc. 113, 37 (1999).
15. Analysis of an energy-resolved spectrum requires knowledge of the potential energy surface in order to apply symmetry arguments since large amplitude motion often affects the observable. On the ultrafast time scale of the experiments considered here large amplitude motion is rarely significant and hence point group symmetry can be used in the majority of cases. In this situation, only the electronic symmetry of the states involved need be known.
16. Experiments currently being set up and initiated to measure femtosecond-resolved PADs are mostly based on photoelectron imaging, from which both complementary observables as well as the (often useful) energy dependence of the PAD are extractable.
17. T. Seideman, J. Chem. Phys. 107, 7859 (1997).
18. S. C. Althorpe and T. Seideman, J. Chem. Phys. 110, 147 (1999).
19. Y. Arasaki et al., Chem. Phys. Lett. 302, 363 (1999).
20. S. C. Althorpe and T. Seideman, J. Chem. Phys. (submitted).
21. T. Seideman and S. C. Althorpe, J. Electron. Spectrosc. Relat. Phenom (in press).
22. Femtosecond photoelectron-photoion coincidence imaging experiments were reported by J. A. Davies, J. E. LeClaire, R. E. Continetti, and C. C. Hayden, J. Chem. Phys. 111, 1 (1999).
23. K. L. Reid, T. A. Field, M. Towrie, and P. Matousek, J. Chem. Phys. 111, 1438 (1999).
24. T. Seideman, J. Chem. Phys. (submitted).
25. Note, however, that while Refs. 7 and 8 exploited the favorable ionization propensity rules of this specific system, here we use it as an experimentally relevant example of what we expect to be a general phenomenon. Hence the complementary ionization correlations of OT (Ref. 8) are not used.
26. See, for instance, H. Petek et al., J. Chem. Phys. 102, 4726 (1994).
27. Closely related to Eqs. (1), (2) (and observable) are so-called fixed-molecule PADs, obtainable from photoion-photoelectron correlation experiments [I. Powis, J. Chem. Phys. 111, 4535 (1999).]. The latter, however, depend on the light polarization in the molecular frame.
28. Equation (3) may have been anticipated since, from the viewpoint of angular momentum algebra, a pump-probe experiment is equivalent to a two-photon transition in the weak field limit.
29. An analogous result was obtained in studies of resonance-enhanced two-photon ionization in the energy domain, K. L. Reid, D. J. Leahy, and R. N. Zare, J. Chem. Phys. 95, 1746 (1991).
30. T. Seideman, J. Chem. Phys. 103, 7887 (1995).
31. B. Friedrich and D. Herschbach, Phys. Rev. Lett. 74, 4623 (1995); H. Sakai el al., J. Chem. Phys. 110, 10235 (1999).
32. B. Friedrich and D. Herschbach, Phys. Rev. Lett. 74, 4623 (1995); H. Sakai el al., J. Chem. Phys. 110, 10235 (1999).
33. P. R. Bunker and P. Jensen, Molecular Symmetry and Spectroscopy (NRC Research Press, Ottawa, 1998), Chap. 3.