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Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed CH4/N2 measurements in binary gas mixtures

Authors

  • Sascha R. Engel,

    1. Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany
    2. Lehrstuhl für Technische Thermodynamik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany
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  • Joseph D. Miller,

    1. Department of Mechanical Engineering, Iowa State University, Ames, IA, USA
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  • Chloe E. Dedic,

    1. Department of Mechanical Engineering, Iowa State University, Ames, IA, USA
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  • Thomas Seeger,

    1. Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany
    2. Lehrstuhl für Technische Thermodynamik, Universität Siegen, Siegen, Germany
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  • Alfred Leipertz,

    1. Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany
    2. Lehrstuhl für Technische Thermodynamik, Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany
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  • Terrence R. Meyer

    Corresponding author
    1. Erlangen Graduate School in Advanced Optical Technologies (SAOT), Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany
    2. Department of Mechanical Engineering, Iowa State University, Ames, IA, USA
    • Correspondence to: Terrence R. Meyer, Department of Mechanical Engineering, Iowa State University, Ames, IA 50011, USA. E-mail: trm@iastate.edu

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  • 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.

Abstract

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.

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