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Issue 40, 2011
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Wavelength-modulated femtosecond stimulated raman spectroscopy—approach towards automatic data processing

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Abstract

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 β-carotene and a similar synthetic aryl carotenoid. The experiments confirm earlier FSRS results on β-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 β-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.

Graphical abstract: Wavelength-modulated femtosecond stimulated raman spectroscopy—approach towards automatic data processing

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Article information


Submitted
23 May 2011
Accepted
24 Aug 2011
First published
12 Sep 2011

Phys. Chem. Chem. Phys., 2011,13, 18123-18133
Article type
Paper

Wavelength-modulated femtosecond stimulated raman spectroscopy—approach towards automatic data processing

M. Kloz, R. V. Grondelle and J. T.M. Kennis, Phys. Chem. Chem. Phys., 2011, 13, 18123
DOI: 10.1039/C1CP21650C

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