Journal
SCIENCE
Volume 334, Issue 6056, Pages 634-639Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1211350
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Funding
- Fannie and John Hertz Foundation
- National Science Foundation
- Stanford Graduate Fellowship
- Air Force Office of Scientific Research [F49620-01-1-0018]
- Department of Energy [DE-FG03-84ER13251]
- National Institutes of Health [GM50730]
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Ultrafast two-dimensional infrared (2D IR) vibrational echo spectroscopy has proven broadly useful for studying molecular dynamics in solutions. Here, we extend the technique to probing the interfacial dynamics and structure of a silica surface-tethered transition metal carbonyl complex-tricarbonyl (1,10-phenanthroline) rhenium chloride-of interest as a photoreduction catalyst. We interpret the data using a theoretical framework devised to separate the roles of structural evolution and excitation transfer in inducing spectral diffusion. The structural dynamics, as reported on by a carbonyl stretch vibration of the surface-bound complex, have a characteristic time of similar to 150 picoseconds in the absence of solvent, decrease in duration by a factor of three upon addition of chloroform, and decrease another order of magnitude for the bulk solution. Conversely, solvent-complex interactions increase the lifetime of the probed vibration by 160% when solvent is applied to the monolayer.
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