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Photoisomerization is a prototypical photophysical and photochemical reaction, the reaction quantum yield depends on its excited-state dynamic. Altering the evolution path of molecular excited states to achieve precise control over photochemical reactions has long been a dream pursued by physicists and chemists. To investigate the effect of femtosecond laser pulse on the ultrafast reaction, the ultrafast photoisomerization of 1,1'-diethyl-2,2'-cyanine iodide (1122C) in methanol was studied using Pump-Dump-Probe spectroscopy. A third femtosecond pulse (Dump) at 1030 nm was introduced into the traditional pump-probe experiment, delayed by 1 ps relative to the initial pump pulse. The recovery of ground state bleaching (GSB) as well as decrease of the Cis product were observed in the Pump-Dump-Probe experiment. It suggests that the Dump pulse successfully promote the initial Trans form to skip the Trans-Cis isomerization pathway in the excited state and return to the ground state directly through stimulated emission. We found that the Cis yield was reduced approximately 12.1% under irradiation of the Dump pulse. Our research has successfully manipulated the quantum yields of a typic ultrafast photoisomerization reaction using femtosecond laser pulse, demonstrating the potential of femtosecond multi-pulse spectroscopy in modifying excited-state evolution pathways and optimizing photochemical reaction yields. This study provides theoretical and technical support for precise control of complex photochemical reactions in the future.
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Keywords:
- femtosecond transient absorption spectroscopy /
- photoisomerization /
- excited state dynamics /
- Pump-Dump-Probe
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