Control of reaction efficiency by two-color two-pulse excitation: Photoisomerization of indocyanine green in condensed phase

In cyanine dye, photoisomerization paths involving multiphoton processes were found by two-color two-pulse correlation of ultrafast transient absorption spectroscopy. The reaction efficiency depended on the interval between two pump pulses, UV and NIR pulses, as well as the fluence of the NIR pulse, but was little dependent on that of the UV pulse. These results indicate that the new photoisomerization paths involve the NIR multiphoton process and/or the UV one-photon process. The difference in two-pulse correlation between positive and negative time regions revealed a new reaction path that had the highest branching ratio of cis isomer to other leuco forms.

54Highlights► Two-color two-pulse correlation in ultrafast transient absorption spectroscopy. ► New photoisomerization paths of ICG including multiphoton process were found. ► Optical orders of UV and NIR pulses in new photoreaction paths were revealed. ► Control of reaction efficiency by delay between pump pulses and their fluences.