This article is from the ECONOS part of the joint special issue on the European Conference on Nonlinear Optical Spectroscopy (ECONOS 2012) with Guest Editors Johannes Kiefer and Peter Radi and the II Italian Conference of the National Group of Raman Spectroscopy and Non-Linear Effects (GISR 2012) with Guest Editor Maria Grazia Giorgini.
Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed CH4/N2 measurements in binary gas mixtures†
Article first published online: 27 FEB 2013
Copyright © 2013 John Wiley & Sons, Ltd.
Journal of Raman Spectroscopy
Special Issue: Joint special issue on the European Conference on Nonlinear Optical Spectroscopy (ECONOS 2012) and the II Italian Conference of the National Group of Raman Spectroscopy and Non-Linear Effects (GISR 2012)
Volume 44, Issue 10, pages 1336–1343, October 2013
How to Cite
Engel, S. R., Miller, J. D., Dedic, C. E., Seeger, T., Leipertz, A. and Meyer, T. R. (2013), Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed CH4/N2 measurements in binary gas mixtures. J. Raman Spectrosc., 44: 1336–1343. doi: 10.1002/jrs.4261
- Issue published online: 22 OCT 2013
- Article first published online: 27 FEB 2013
- Manuscript Accepted: 9 JAN 2013
- Manuscript Revised: 8 JAN 2013
- Manuscript Received: 8 OCT 2012
- U.S. National Science Foundation. Grant Number: CBET-1056006
- German Research Foundation (DFG)
- National Science Foundation Graduate Fellowship Program
- coherent anti-Stokes Raman scattering;
- ultrafast spectroscopy;
- concentration measurement;
- gas sensing
Hybrid femtosecond/picosecond (fs/ps) vibrational coherent anti-Stokes Raman scattering was demonstrated for high-speed, in-situ measurements of CH4/N2 mole fractions in binary gas mixtures with temporal nonresonant suppression. A single broadband, 100-fs laser source was used to simultaneously excite CH4 and N2 vibrational Raman transitions, characterized by a spectral separation of ~584 cm−1, followed by frequency-domain detection with a time-delayed ps probe pulse. In this manner, the temporal evolution of the nonresonant background and vibrational wavepackets of CH4 and N2 could be evaluated to maximize signal and minimize interferences. A typical accuracy of ~95% was achieved for experimental CH4 mole fractions between 0.02 and 0.70, and a precision of ~4% was achieved by maximizing relative excitation energy through induced chirp in the pump and Stokes pulses. It was further shown that mole-fraction measurements were not affected by variations in bi-molecular broadened linewidths over a wide range of mixture fractions. Copyright © 2013 John Wiley & Sons, Ltd.