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Two-Photon Excited State Dynamics of Dark Valence, Rydberg, and Superexcited States in 1,3-Butadiene
Stockholm University, Faculty of Science, Department of Physics. National Research Council Canada.
2014 (English)In: Journal of Physical Chemistry Letters, ISSN 1948-7185, Vol. 5, no 3, 560-565 p.Article in journal (Refereed) Published
Abstract [en]

Two-photon absorption in systems with parity permits access to states that cannot be prepared by one-photon absorption. Here we present the first time-resolved photoelectron spectroscopy study using this technique, applied to 1,3-butadiene, in which we investigated the dynamics of its dark valence, Rydberg, and superexcited states. The dark valence state dynamics are accessed via the Rydberg manifold, excited by two photons of 400 nm. We find that the 'dark' 2(1)A(g) state populated in this manner has a much longer lifetime than when accesses via the 1(1)B(u) 'bright' valence state when populated by one photon of 200 nm. In addition, we compared the dynamics of the 3s pi- and 3d pi-Rydberg states. These Rydberg states relax to the valence manifold on a subpicosecond time scale, with the 3s pi-Rydberg state decay rate being larger due to a stronger valence-Rydberg mixing. Finally, we investigated superexcited valence states that fragment or autoionize within 200 fs, likely without involving Rydberg states.

Place, publisher, year, edition, pages
2014. Vol. 5, no 3, 560-565 p.
National Category
Physical Sciences
URN: urn:nbn:se:su:diva-102076DOI: 10.1021/jz402725uISI: 000331153600029OAI: diva2:708433
The Wenner-Gren Foundation


Available from: 2014-03-27 Created: 2014-03-26 Last updated: 2014-03-27Bibliographically approved

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Schalk, Oliver
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