Author(s):

Bhaskar A (Bhaskar, Ajit), Ramakrishna G (Ramakrishna, Guda), Lu ZK (Lu, Zhikuan), Twieg R (Twieg, Robert), Hales JM (Hales, Joel M.), Hagan DJ (Hagan, David J.), Van Stryland E (Van Stryland, Eric), Goodson T (Goodson, Theodore, III)

Abstract:

Novel alkene and alkyne branched structures have been synthesized, and their two-photon absorption (2PA) properties are reported. This series of alkene and alkyne trimer systems tests the mechanistic approach for enhancing the 2PA process which is usually dictated by the pi-bridging, delocalization length, and corresponding charge transfer on the 2PA cross sections. The results suggest that alkene branched systems have higher 2PA cross sections. While steady-state absorption and emission measurements were not successful in predicting the observed trend of 2PA cross sections, time-resolved measurements have explained the trends observed. It was found that, upon photoexcitation, there is an ultrafast charge localization to an intramolecular charge-transfer (ICT) state, followed by the presence of a solvent and conformationally relaxed ICT state ' in these branched systems.