Collision-induced Raman scattering by rare-gas atoms: The isotropic spectrum of Ne-Ne and its mean polarizability.

We report the room-temperature isotropic collision-induced light scattering spectrum of Ne-Ne over a wide interval of Raman shifts, and we compare it with the only available experimental spectrum for that system as well as with spectra calculated quantum-mechanically with the employ of advanced ab initio-computed data for the incremental mean polarizability. The spectral range previously limited to 170 cm(-1) is now extended to 485 cm(-1) allowing us to successfully solve the inverse-scattering problem toward an analytic model for the mean polarizability that perfectly matches our measurements. We also report the depolarization ratio of the scattering process, lingering over the usefulness of this property for more stringent checks between the various polarizability models.

[1]  S. Dixneuf,et al.  Collision-induced Raman scattering and the peculiar case of neon: anisotropic spectrum, anisotropy, and the inverse scattering problem. , 2015, The Journal of chemical physics.

[2]  F. Grandinetti.  Neon behind the signs. , 2013, Nature chemistry.

[3]  J Burgdörfer,et al.  Delay in Photoemission , 2010, Science.

[4]  S. Dixneuf,et al.  Anisotropic collision-induced Raman scattering by Ne-Ne: Evidence for a nonsmooth spectral wing , 2009 .

[5]  S. Dixneuf,et al.  Isotropic and anisotropic collision-induced Raman scattering by monoatomic gas mixtures: Ne-Ar , 2009 .

[6]  Jürg Hutter,et al.  Ab Initio Molecular Dynamics: Basic Theory and Advanced Methods , 2009 .

[7]  L. Frommhold.  Collision‐Induced Scattering of Light and the Diatom Polarizabilities , 2007 .

[8]  S. Dixneuf,et al.  Induced anisotropy of Ar2: a state-of-the-art semiempirical model. , 2005, The Journal of chemical physics.

[9]  N. Makri,et al.  Quantum dynamics in simple fluids. , 2004, The Journal of chemical physics.

[10]  C. Hättig,et al.  Ab initio calculation of the refractivity and hyperpolarizability second virial coefficients of neon gas , 2003 .

[11]  M. Chrysos,et al.  Absolute isotropic spectral intensities in collision-induced light scattering by helium pairs over a large frequency domain , 2000 .

[12]  G. Maroulis.  Computational Aspects of Interaction Hyperpolarizability Calculations. A Study on H2···H2, Ne···HF, Ne···FH, He···He, Ne···Ne, Ar···Ar, and Kr···Kr† , 2000 .

[13]  J. Olsen,et al.  The effect of intermolecular interactions on the electric properties of helium and argon. I. Ab initio calculation of the interaction induced polarizability and hyperpolarizability in He2 and Ar2 , 1999 .

[14]  H. Koch,et al.  Ab initio calculation of the frequency-dependent interaction induced hyperpolarizability of Ar2 , 1999 .

[15]  Z. Rudzikas.  Theoretical atomic spectroscopy , 1997 .

[16]  S. Goldman,et al.  The pair polarizability of argon , 1996 .

[17]  M. Chrysos,et al.  Quantum analysis of absolute collision‐induced scattering spectra from bound, metastable and free Ar diatoms , 1996 .

[18]  M. Chrysos,et al.  Quantum description of high-frequency Raman scattering from pairs of argon atoms , 1996 .

[19]  Lothar Frommhold,et al.  Collision-induced absorption in gases , 2006 .

[20]  R. A. Aziz,et al.  The Ne-Ne interatomic potential revisited , 1989 .

[21]  T. Bose,et al.  Refractivity virial coefficients of C2H4 and C2H4–Ar mixtures , 1988 .

[22]  R. Pecora.  Dynamic Light Scattering , 1985 .

[23]  R. Coulon,et al.  Détermination expérimentale des coefficients du viriel de la réfractivité des gaz : étude de l'argon , 1981 .

[24]  M. Proffitt,et al.  Collision-induced Raman spectra and diatom polarizabilities of the rare gases – an update , 1981 .

[25]  R. D. Cowan,et al.  The Theory of Atomic Structure and Spectra , 1981 .

[26]  M. Proffitt,et al.  Collision-induced Raman spectra of neon and the diatom polarizability , 1980 .

[27]  M. Lallemand,et al.  Variation of the polarizability of noble gases with density , 1977 .

[28]  M. Lallemand,et al.  Evolution of the Clausius–Mossotti function of noble gases and nitrogen, at moderate and high density, near room temperature , 1976 .

[29]  A. D. Buckingham,et al.  The density dependence of the refractivity of gases , 1974, Proceedings of the Royal Society of London. A. Mathematical and Physical Sciences.

[30]  M. H. Hart.  A possible atmosphere for Pluto , 1974 .

[31]  R. Cole,et al.  Dielectric Constants of Imperfect Gases. III. Atomic Gases, Hydrogen, and Nitrogen , 1967 .