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Femtosecond time-resolved ionization spectroscopy of Na3(B) and the question of the geometric phase

✍ Scribed by J. Schön; H. Köppel

Publisher
Elsevier Science
Year
1994
Tongue
English
Weight
806 KB
Volume
231
Category
Article
ISSN
0009-2614

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✦ Synopsis

The femtosecond time-resolved ionization spectrum of the B-state of Na, has been studied theoretically, taking two nuclear degrees of freedom into account (bending mode and pseudorotation ). Special emphasis is put on a comparison between different approaches to the pseudorotational dynamics of Na,(B) proposed earlier in the literature: a Jahn-Teller treatment invoked in the original work versus a pseudo-Jahn-Teller treatment advanced in later studies. The time-dependent wave-packet dynamics is found to differ drasticalty in the two cases although it proceeds on (visually) the same potentiat energy surface. This is interpreted as a consequence of the geometric phase which is nontrivial only in the Jahn-Teller case. A low-energy peak in the Fourier transform of the pump-probe spectrum of Baumert et al. (Chem. Phys. Letters 209 ( 1993) 29) is tentatively interpreted as evidence in favour of the pseudo-Jahn-Teller mechanism.

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