Journal
JOURNAL OF RAMAN SPECTROSCOPY
Volume 42, Issue 10, Pages 1883-1890Publisher
WILEY
DOI: 10.1002/jrs.2996
Keywords
ultrafast Raman loss spectroscopy; stimulated Raman scattering; higher order nonlinear process; fluorescence rejection; vibrational structure
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Funding
- Department of Science and Technology (DST), Govt. of India
- Indian Institute of Science (IISc)
- DST
- Council of Scientific and Industrial Research (CSIR), Govt. of India
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In this paper, we report on the concept and the design principle of ultrafast Raman loss spectroscopy (URLS) as a structure-elucidating tool. URLS is an analogue of stimulated Raman scattering (SRS) but more sensitive than SRS with better signal-to-noise ratio. It involves the interaction of two laser sources, namely, a picosecond (ps) Raman pump pulse and a white-light (WL) continuum, with a sample, leading to the generation of loss signals on the higher energy (blue) side with respect to the wavelength of the Raman pump unlike the gain signal observed on the lower energy (red) side in SRS. These loss signals are at least 1.5 times more intense than the SRS signals. An experimental study providing an insight into the origin of this extra intensity in URLS as compared to SRS is reported. Furthermore, the very requirement of the experimental protocol for the signal detection to be on the higher energy side by design eliminates the interference from fluorescence, which appears on the red side. Unlike CARS, URLS signals are not precluded by the non-resonant background and, being a self-phase-matched process, URLS is experimentally easier. Copyright (C) 2011 John Wiley & Sons, Ltd.
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