Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 123, Issue 30, Pages 6463-6471Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.9b06427
Keywords
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Funding
- Scientific Instrumentation Fund of the Chinese Academy of Sciences [Y2201228]
- National Natural Science Foundation of China [21573243, 21327802, 11674101, 21473212]
- Science & Technology Programs of Jiangxi Provincial Department of Education [GJJ180235]
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It has been a long-lasting debate whether indigo undergoes excited-state proton transfer and how this contributes to its photostability. A prevailing point of view is that a sub-picosecond excited-state intramolecular single proton transfer occurs; however, it has been studied mostly under dilute solution conditions. In this work, excited-state structural dynamics of indigo oligomers formed at millimolar concentration in dimethyl sulfoxide is investigated using femtosecond visible pump spectroscopy, infrared and visible probe spectroscopies, and steady-state infrared and fluorescence spectroscopies. Experimental evidence indicates the presence of transient intermolecular electronic excited-state proton transfer, which is supported by quantum-chemistry computations. The formed enol species disappears with a time constant of 200-300 fs, followed by a relatively slow nonradiative relaxation to the electronic ground state. Our results reveal new photochemistry of indigo particularly in its oligomeric state.
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