Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 13, Issue 40, Pages 18123-18133Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c1cp21650c
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Funding
- Chemical Sciences council of the Netherlands Organization for Scientific Research (NWO-CW)
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A new wavelength modulator based on a custom-made chopper blade and a slit placed in the Fourier plane of a pulse shaper was used to detect explicitly the first derivative of the time-resolved femtosecond stimulated Raman spectroscopy (FSRS) signals. This approach resulted in an unprecedented reduction of the non-coherent background that results from population transfer by the Raman pump inherent to FSRS experiments. The method of Fourier peak filtering was implemented as a powerful tool for reducing both the remaining non-coherent and coherent background associated with FSRS experiments. The method was demonstrated on beta-carotene and a similar synthetic aryl carotenoid. The experiments confirm earlier FSRS results on beta-carotene but suggest some reinterpretation. Strong bleaching signals of ground state vibrations were observed and interpreted as an inseparable part of the time-resolved FSRS experiment. New long-lived Raman features were observed in b-carotene and the synthetic aryl carotenoid and assigned to a combination of conformational changes and solvent rearrangement. More complex wavelength modulation methods are proposed in the development of more robust FSRS experiments.
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