Watching ultrafast barrierless excited-state isomerization of pseudocyanine in real time |
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Authors: | Dietzek Benjamin Yartsev Arkady Tarnovsky Alexander N |
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Institution: | Department of Chemical Physics, Lund University, P.O. Box 124, 22100 Lund, Sweden. |
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Abstract: | The photoinduced excited-state processes in 1,1'-diethyl-2,2'-cyanine iodine are investigated using femtosecond time-resolved pump-probe spectroscopy. Using a broad range of probe wavelengths, the relaxation of the initially prepared excited-state wavepacket can be followed down to the sink region. The data directly visualize the directed downhill motion along the torsional reaction coordinate and suggest a barrierless excited-state isomerization in the short chain cyanine dye. Additionally, ultrafast ground-state hole and excited-state hole replica broadening is observed. While the narrow excited-state wavepacket broadens during pump-probe overlap, the ground-state hole burning dynamics takes place on a significantly longer time-scale. The experiment reported can be considered as a direct monitoring of the shape and the position of the photoprepared wavepacket on the excited-state potential energy surface. |
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