Collision effects in the nonlinear Raman response of liquid carbon disulfide

Jansen, Thomas l. C.; Swart, Marcel; Jensen, Lasse; van Duijnen, Piet Th.; Snijders, Jaap G.; Duppen, Koos
February 2002
Journal of Chemical Physics;2/22/2002, Vol. 116 Issue 8, p3277
Academic Journal
A model of the polarizability of carbon disulfide dimers was constructed, using polarizabilities from accurate time-dependent density functional theory calculations as reference. This direct reaction field model takes dipole-induced dipole effects, induced multipole effects and effects due to the overlap of the electronic clouds into account in an approximate way. The importance of the induced multipole and the overlap effects is investigated. This polarizability model is subsequently used to calculate the third-order time-domain Raman response of liquid carbon disulfide. These results are compared to experimental data and earlier calculated response in which only dipole-induced dipole effects on the polarizability were included. The multipole effects are found to give a significant contribution to the subpico second part of the third-order Raman response.


Related Articles

  • Many-body effects in the stimulated Raman response of binary mixtures: A comparison between theory and experiment. Jansen, Thomas l. C.; Pugzlys, Audrius; Crı⁁ngus¸, Gheorghe Dan; Snijders, Jaap G.; Duppen, Koos // Journal of Chemical Physics;6/1/2002, Vol. 116 Issue 21, p9383 

    The subpicosecond dynamics of binary mixtures of carbon disulfide and alkane have been studied using third-order time-resolved Raman techniques. Both the anisotropic and the isotropic responses were investigated. These depend differently on many-body contributions to the first-order...

  • The resonance Raman excitation profile of violaxanthin. Hoskins, L. C.; McCarthy, M. C. // Journal of Chemical Physics;8/1/1986, Vol. 85 Issue 3, p1322 

    The resonance Raman excitation profiles for the ν1, ν2, and ν3 vibrations of violaxanthin in acetone, toluene, and carbon disulfide solvents have been measured. The results are interpreted in terms of a three-mode vibrational theory which includes both homogeneous and inhomogeneous...

  • Temperature-dependent resonance Raman profiles of β-carotene in carbon disulfide. Lee, S. A.; Chan, C. K.; Page, J. B.; Walker, C. T. // Journal of Chemical Physics;3/1/1986, Vol. 84 Issue 5, p2497 

    Resonance Raman (RR) profiles of the 1005, 1155, and 1525 cm-1 modes of β-carotene dissolved in carbon disulfide have been measured at room temperature and at 172 K. Previous studies, based upon room temperature measurements, have indicated that inhomogeneous (i.e., site) broadening may be...

  • High pressure Raman study of solid CS2. Bolduan, F.; Hochheimer, H. D.; Jodl, H. J. // Journal of Chemical Physics;6/15/1986, Vol. 84 Issue 12, p6997 

    Solid molecular CS2 is investigated in a diamond anvil cell in the temperature and pressure range of 6–300 K and 0–20 GPa, respectively, by means of Raman spectroscopy. The pressure dependence of external and internal vibrational frequencies is determined, and used to draw...

  • Polarized and depolarized Raman spectra of liquid carbon disulfide in the pressure range 0–10 kbar. II. Reorientational and vibrational relaxation. Ikawa, S.; Whalley, Edward // Journal of Chemical Physics;2/15/1987, Vol. 86 Issue 4, p1836 

    The effect of pressure on the reorientational and the vibrational phase correlation times of liquid carbon disulfide has been determined up to 10 kbar at 295 K from the widths of the isotropic and anisotropic components of the Raman ν1 band. The reorientational correlation time increases with...

  • A resonance Raman intensity study of electronic spectral broadening mechanisms in CS2/cyclohexane. Myers, Anne B.; Li, Bulang; Ci, Xiaopei // Journal of Chemical Physics;8/15/1988, Vol. 89 Issue 4, p1876 

    Complete resonance Raman spectra, including absolute cross sections, have been measured for CS2 in cyclohexane using four excitation wavelengths from 223 to 204 nm, on resonance with the strongly allowed S3←S0 electronic transition. Absolute intensities have also been measured in CS2 vapor...

  • Separation of temperature and density effects on collision-induced Rayleigh and Raman line shapes of liquid carbon disulfide. Hegemann, B.; Jonas, J. // Journal of Chemical Physics;4/1/1985, Vol. 82 Issue 7, p2845 

    Quantitative results for the separate temperature and density effects on collision-induced scattering (CIS) line shapes for the dense molecular fluid CS2 are presented for the temperature range T=293–353 K and density range ρ=1.25–1.48 g cm-3. The depolarized Rayleigh scattering...

  • Non-Lorentzian depolarized Raman line shapes in n-pentanol. Di Fabrizio, E.; Nardone, M.; Nucara, A.; Gallo, P.; Ruocco, G. // Journal of Chemical Physics;11/1/1992, Vol. 97 Issue 9, p6136 

    High resolution depolarized Raman spectra of n-pentanol in the -30 to 60° C temperature range are reported. The spectra appear as a continuously decreasing line shape centered at zero frequency. A quantitative analysis of this line shape shows a high frequency exponential tail, which can...

  • Interaction induced effects in the nonlinear Raman response of liquid CS[sub 2]: A finite field nonequilibrium molecular dynamics approach. Jansen, Thomas l. C.; Snijders, Jaap G.; Duppen, Koos // Journal of Chemical Physics;6/22/2001, Vol. 114 Issue 24 

    The third- and fifth-order time-domain Raman responses of liquid carbon disulfide have been calculated, taking local field effects into account through the dipole-induced dipole approximation to the polarizability. The third-order response is shown to be in excellent agreement with experimental...


Read the Article


Sorry, but this item is not currently available from your library.

Try another library?
Sign out of this library

Other Topics