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Coherent Raman Scattering in High-Pressure/High Temperature Fluids: An Overview

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Coherent Raman Spectroscopy

Part of the book series: Springer Proceedings in Physics ((SPPHY,volume 63))

Abstract

The present understanding of high-pressure/high-temperature dense-fluid behavior is derived almost exclusively from hydrodynamic and thermodynamic measurements. Such results average over the microscopic aspects of the materials and are, therefore, insufficient for a complete understanding of fluid behavior. At present, dense-fluid models can be verified only to the extent that they agree with the macroscopic measurements. Recently, using stimulated Raman scattering, Raman induced Kerr effect scattering, and coherent anti-Stokes Raman scattering, we have been able to probe some of the microscopic phenomenology of these dense fluids. In this paper, we discuss primarily the use of CARS in conjunction with a two-stage light-gas gun to obtain vibrational spectra of shock-compressed liquid N2, O2, CO, their mixtures, CH3NO2, and N2O. These experimental spectra are compared to synthetic spectra calculated using a semiclassical model for CARS intensities and best fit vibrational frequencies, peak Raman susceptibilities, and Raman linewidths. For O2, the possibility of resonance enhancement from collision-induced absorption is addressed. Shifts in the vibrational frequencies reflect the influence of increased density and temperature on the intramolecular motion. The derived parameters suggest thermal equilibrium of the vibrational levels is established less than a few nanoseconds after shock passage. Vibrational temperatures are obtained that agree with those derived from equation-of-state calculations. Measured linewidths suggest that vibrational dephasing times have decreased to subpicosecond values at the highest shock pressures.

This work was supported by the US Department of Energy

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Authors and Affiliations

  1. Los Alamos National Laboratory, 87545, Los Alamos, NM, USA

    S. C. Schmidt & D. S. Moore

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  1. S. C. Schmidt
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Editors and Affiliations

  1. Max-Planck-Institut für Biophysikalische Chemie, Abteilung Laserphysik, Am Fassberg, W-3400, Göttingen, Germany

    Gerd. Marowsky

  2. General Physics Institute, Academy of Sciences, Vavilov Street 38, SU-117942, Moscow, USSR

    Valery V. Smirnov

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Schmidt, S.C., Moore, D.S. (1992). Coherent Raman Scattering in High-Pressure/High Temperature Fluids: An Overview. In: Marowsky, G., Smirnov, V.V. (eds) Coherent Raman Spectroscopy. Springer Proceedings in Physics, vol 63. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-77194-1_25

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  • DOI: https://doi.org/10.1007/978-3-642-77194-1_25

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