NDLI: Hydrogen bond breaking probed with multidimensional stimulated vibrational echo correlation spectroscopy

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Hydrogen bond breaking probed with multidimensional stimulated vibrational echo correlation spectroscopy

Content Provider	Semantic Scholar
Author	Asbury, John B. Steinel, Tobias Stromberg, Christopher J. Gaffney, Kelly J. Piletic, Ivan R. Fayer, Michael D.
Copyright Year	2003
Abstract	H bond population dynamics are extricated with exceptional detail using ultrafast (<50 fs) IR multidimensional stimulated vibrational echo correlation spectroscopy with full phase information and frequency resolved IR pump-probe expts. performed on the hydroxyl stretch of MeOH-OD oligomers in CCl4. H bond breaking makes it possible to acquire data for times much greater than the hydroxyl stretch vibrational lifetime. The correlation spectra and detailed calcns. demonstrate that vibrational relaxation leads to H bond breaking for oligomers that have hydroxyl stretch frequencies on the low energy (red) side of the hydroxyl stretch spectrum, the spectral region that is assocd. with the strongest H bonds. Frequency resolved pump-probe data support the conclusions drawn from the correlation spectra. Using a global fit to the pump-probe spectra, in conjunction with assignments made possible through the correlation spectra, the residual ground state and photoproduct of H bond breaking were prepd. near their thermal equil. distribution. The spectrum of the H bond breaking photoproduct and the residual ground state approach the steady-state temp. difference spectrum on the tens of picoseconds time scale, indicating the system thermalizes on this time scale. [on SciFinder(R)]
Starting Page	12981
Ending Page	12997
Page Count	17
File Format	PDF HTM / HTML
DOI	10.1063/1.1627762
Volume Number	119
Alternate Webpage(s)	http://web.stanford.edu/group/fayer/articles/305.pdf
Alternate Webpage(s)	https://doi.org/10.1063/1.1627762
Language	English
Access Restriction	Open
Content Type	Text
Resource Type	Article

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