Journal
JOURNAL OF RAMAN SPECTROSCOPY
Volume 44, Issue 3, Pages 433-439Publisher
WILEY
DOI: 10.1002/jrs.4215
Keywords
femtosecond stimulated Raman scattering; thermometry; picosecond time resolution
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Funding
- US Department of Energy through the Los Alamos Laboratory Directed Research and Development program and Science Campaign 2: High Explosives Science
- Defense Threat Reduction Agency Basic Research program
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We have previously demonstrated the capability of femtosecond stimulated Raman scattering (FSRS) data to measure the temperature (T) of condensed matter at the molecular vibrational level. [Phys. Rev. Lett. 2011, 107, 43001] In this paper, we expand the theory for the FSRS temperature dependence by considering the effects of an isolated change of T as well as a coupled change of T and chemical concentration. We point out that the origin of the temperature sensitivity of the Stokes to anti-Stokes ratio of FSRS lies in the exponential nonlinearity of the gain and loss. We establish that FSRS of two Raman modes can be used to simultaneously determine the vibrational temperature and the change in concentration of the species contributing to those two modes. Single-shot experimental results using FSRS are presented to demonstrate over four orders of magnitude higher efficiency than spontaneous Raman in small volume samples with picosecond resolution. Copyright (c) 2012 John Wiley & Sons, Ltd.
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