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Introductory Lecture. Probing wavepacket dynamics with femtosecond energy- and angle-resolved photoelectron spectroscopy

Takatsuka, Kazuo and Arasaki, Yasuki and Wang, Kwanghsi and McKoy, Vincent (2000) Introductory Lecture. Probing wavepacket dynamics with femtosecond energy- and angle-resolved photoelectron spectroscopy. Faraday Discussions, 115 . pp. 1-15. ISSN 1359-6640. doi:10.1039/b002739l.

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Several recent studies have demonstrated how well-suited femtosecond time-resolved photoelectron spectra are for mapping wavepacket dynamics in molecular systems. Theoretical studies of femtosecond photoelectron spectra which incorporate a robust description of the underlying photoionization dynamics should enhance the utility of such spectra as a probe of wavepackets and of the evolution of electronic structure. This should be particularly true in regions of avoided crossings where the photoionization amplitudes and electronic structure may evolve rapidly with geometry. In this paper we present the results of studies of energy- and angle-resolved femtosecond photoelectron spectra for wavepackets in the diatomic systems, Na2 and NaI. Both cases involve motion through regions of avoided crossings. In Na2, however, wavepacket motion occurs on a single adiabatic potential with an inner and outer well and a barrier between them, while in NaI wavepackets move on the nonadiabatically coupled covalent (NaI) and ionic (Na+I–) potentials. Results of these studies will be used to illustrate the insight into wavepacket dynamics that time-resolved photoelectron spectra provide. For example, in the case of NaI these angle-resolved photoelectron spectra seem to offer some promise for probing real-time dynamics of intramolecular electron transfer occurring in the crossing region of the ionic and covalent states.

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Additional Information:The journal is © The Royal Society of Chemistry 2000. Received 6th April 2000. Published on the Web 15th June 2000. This work was supported by a grant from the Ministry of Education, Science and Culture (Japan) and the National Science Foundation (USA).
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Ministry of Education, Culture, Sports, Science and Technology (MEXT)UNSPECIFIED
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Deposited On:01 May 2008
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