Rayleigh-Brillouin scattering in SF6 in the kinetic regime

Abstract Rayleigh-Brillouin spectral profiles are measured with a laser-based scatterometry setup for a 90° scattering angle at a high signal-to-noise ratio (r.m.s. noise below 0.15% w.r.t. peak intensity) in sulfur-hexafluoride gas for pressures in the range 0.2–5 bar and for a wavelength of λ = 403.0  nm. The high quality data are compared to a number of light scattering models in order to address the effects of rotational and vibrational relaxation. While the vibrational relaxation rate is so slow that vibration degrees of freedom remain frozen, rotations relax on time scales comparable to those of the density fluctuations. Therefore, the heat capacity, the thermal conductivity and the bulk viscosity are all frequency-dependent transport coefficients. This is relevant for the Tenti model that depends on the values chosen for these transport coefficients. This is not the case for the other two models considered: a kinetic model based on rough-sphere interactions, and a model based on fluctuating hydrodynamics. The deviations with the experiment are similar between the three different models, except for the hydrodynamic model at pressures p ≲ 2 bar . As all models are in line with the ideal gas law, we hypothesize the presence of real gas effects in the measured spectra.

[1]  Z. Gu,et al.  Temperature-dependent bulk viscosity of nitrogen gas determined from spontaneous Rayleigh-Brillouin scattering. , 2013, Optics letters.

[2]  Richard B Miles,et al.  Coherent Rayleigh-Brillouin scattering. , 2002, Physical review letters.

[3]  T. G. Cowling,et al.  The mathematical theory of non-uniform gases , 1939 .

[4]  G. Benedek,et al.  Spectrum of Light Scattered from Thermal Fluctuations in Gases , 1966 .

[5]  B Witschas Analytical model for Rayleigh-Brillouin line shapes in air. , 2011, Applied optics.

[6]  Stampanoni-Panariello,et al.  Electrostrictive generation of nonresonant gratings in the gas phase by multimode lasers. , 1995, Physical review. A, Atomic, molecular, and optical physics.

[7]  Benjamin Chu,et al.  Rayleigh–Brillouin scattering of gases with internal relaxation , 1976 .

[8]  T. A. Wiggins,et al.  Rayleigh–Brillouin scattering from methane , 1976 .

[9]  Jacques Bordé,et al.  Vibration-rotation molecular constants for the ground and (ν3 = 1) states of 32SF6 from saturated absorption spectroscopy , 1987 .

[10]  Mikhail N. Shneider,et al.  Power spectrum of coherent Rayleigh-Brillouin scattering in carbon dioxide , 2005 .

[11]  P. Barker,et al.  Frequency-resolved coherent rayleigh scattering at low densities with nearly-degenerate four-wave mixing , 2000 .

[12]  L. E. Sutton,et al.  Investigation by electron diffraction of the molecular structures of sulphur hexafluoride, sulphur tetrafluoride, selenium hexafluoride and selenium tetrafluoride , 1963 .

[13]  Lord Rayleigh F.R.S. XXXIV. On the transmission of light through an atmosphere containing small particles in suspension, and on the origin of the blue of the sky , 1899 .

[14]  L. Brillouin Diffusion de la lumière et des rayons X par un corps transparent homogène - Influence de l'agitation thermique , 1922 .

[15]  N. Dam,et al.  Coherent and spontaneous Rayleigh-Brillouin scattering in atomic and molecular gases and gas mixtures , 2010 .

[16]  R. Kapral,et al.  Light-Scattering Experiments and Generalized Transport Coefficients , 1973 .

[17]  J. McCoubrey,et al.  Intermolecular forces in quasi-spherical molecules , 1957 .

[18]  Robert D. Trengove,et al.  The Viscosity of Carbon Dioxide, Methane, and Sulfur Hexafluoride in the Limit of Zero Density , 1987 .

[19]  E. A. Mason,et al.  Equilibrium and Transport Properties of Eleven Polyatomic Gases At Low Density , 1987 .

[20]  Benjamin Witschas,et al.  Rayleigh-Brillouin scattering profiles of air at different temperatures and pressures. , 2013, Applied optics.

[21]  C. D. Boley,et al.  Kinetic Models and Brillouin Scattering in a Molecular Gas , 1972 .

[22]  Luda Wang,et al.  Selective molecular sieving through porous graphene. , 2012, Nature nanotechnology.

[23]  J. Kestin,et al.  Thermal conductivity of sulfur hexafluoride , 1985 .

[24]  Z. Gu,et al.  A Rayleigh-Brillouin scattering spectrometer for ultraviolet wavelengths. , 2012, Review of Scientific Instruments.

[25]  Barker,et al.  Coherent rayleigh scattering , 2000, Physical review letters.

[26]  Wolfgang Wagner,et al.  A Reference Equation of State for the Thermodynamic Properties of Sulfur Hexafluoride (SF6) for Temperatures from the Melting Line to 625K and Pressures up to 150MPa , 2009 .

[27]  Z. Gu,et al.  Rayleigh-Brillouin scattering of carbon dioxide. , 2014, Optics letters.

[28]  Hao Li,et al.  Analysis of Rayleigh-Brillouin spectral profiles and Brillouin shifts in nitrogen gas and air. , 2014, Optics express.

[29]  K. Sakai,et al.  Rotational relaxation in H2 gas observed with optical beating Brillouin spectroscopy , 2009 .

[30]  Hajime Tanaka,et al.  Superheterodyne light beating spectroscopy for Rayleigh–Brillouin scattering using frequency-tunable lasers , 2002 .

[31]  W. Ubachs,et al.  Direct measurement of the Rayleigh scattering cross section in various gases , 2005 .

[32]  Z. Gu,et al.  A systematic study of Rayleigh-Brillouin scattering in air, N₂, and O₂ gases. , 2014, The Journal of chemical physics.

[33]  Egon Hassel,et al.  Viscosity measurements on gaseous sulfur hexafluoride , 2005 .

[34]  W. Marques Light scattering from extended kinetic models: polyatomic ideal gases , 1999 .

[35]  A S de Wijn,et al.  Coherent Rayleigh-Brillouin scattering measurements of bulk viscosity of polar and nonpolar gases, and kinetic theory. , 2010, The Journal of chemical physics.

[36]  M. Cramer Numerical estimates for the bulk viscosity of ideal gases , 2012 .

[37]  C. Boley,et al.  On the Kinetic Model Description of Rayleigh–Brillouin Scattering from Molecular Gases , 1974 .

[38]  She,et al.  Stimulated Rayleigh-Brillouin gain spectroscopy. , 1985, Physical review. A, General physics.

[39]  R. P. Sandoval,et al.  Rayleigh-Brillouin spectra in molecular nitrogen , 1976 .

[40]  N. Clark,et al.  Observation of a Frequency-Dependent Thermal Conductivity in a Polyatomic Gas , 1972 .

[41]  L. Bartell,et al.  STRUCTURES OF HEXACOORDINATE COMPOUNDS OF MAIN-GROUP ELEMENTS Part III. An electron diffraction study of SF6 , 1978 .