Femtosecond infrared pump-stimulated Raman probe spectroscopy: the first application of the method to studies of vibrational relaxation pathways in the liquid HDO/D2O system.
Phys Chem Chem Phys
; 21(31): 16895-16904, 2019 Aug 21.
Article
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| MEDLINE
| ID: mdl-31215570
ABSTRACT
We have proposed and constructed a setup for a novel method of ultrafast vibrational spectroscopy femtosecond infrared pump-stimulated Raman probe spectroscopy. This is the first time-resolved spectroscopy providing simultaneously a sub-100 fs time resolution, a spectral resolution better than 10 cm-1 and a spectral window covering an extremely broad range of molecular vibrations (at least 200-4000 cm-1) with a "single laser shot". The new method was applied to study vibrational relaxation pathways in the liquid HDO/D2O system. We determined the lifetimes of OH stretching vibrations to be in the range 310-500 fs depending on the isotopic dilution, which is in good agreement with the results from pump-probe femtosecond infrared spectroscopy. Moreover, we observed a strong coupling of OH stretch to OD stretch vibrations and possibly also to the librational modes of water.
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2019
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Article