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NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. For the publisher's version, please access the DOI link below./ Pour consulter la version de l'éditeur, utilisez le lien DOI ci-dessous.http://doi.org/10.1021/jz402725uAccess and use of this website and the material on it are subject to the Terms and Conditions set forth at Two-photon excited state dynamics of dark valence, rydberg, and superexcited states in 1,3-butadiene Schalk, Oliver; Boguslavskiy, Andrey E.; Stolow, Albert http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/droits L'accès à ce site Web et l'utilisation de son contenu sont assujettis aux conditions présentées dans le site LISEZ CES CONDITIONS ATTENTIVEMENT AVANT D'UTILISER CE SITE WEB.
NRC Publications Record / Notice d'Archives des publications de CNRC:http://nparc.cisti-icist.nrc-cnrc.gc.ca/eng/view/object/?id=eea29a58-f58d-4ead-8935-0ac01bf7dbef http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/voir/objet/?id=eea29a58-f58d-4ead-8935-0ac01bf7dbef ABSTRACT: 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 3sπ-and 3dπ-Rydberg states. These Rydberg states relax to the valence manifold on a subpicosecond time scale, with the 3sπ-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.