Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 132, Issue 37, Pages 12784-12785Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja1043853
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Funding
- National Science Foundation [CHE-0748501]
- University of Michigan
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [748501] Funding Source: National Science Foundation
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We present the first implementation of transient vibrational Stark-effect spectroscopy as an ultrafast probe of solvation dynamics. The method is applied to the phototriggered intramolecular charge-transfer reaction of Betaine-30, where the vibrational Stark shifts of the nearby solvent molecules-arising from the change in the electrostatic environment-are measured using a three-pulse photon echo probe. This new experiment provides a direct subpicosecond measure of the chromophore's excited-state dynamics and back electron transfer as viewed from the solvent's perspective. We develop a simple ab initio model that offers semiquantitative prediction of the experimental Stark shifts.
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