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A temperature-dependent, low-frequency Raman study for a strong and a fragile glass-forming liquid is reported in order to elucidate the frequency and temperature sensitivity of the depolarization ratio spectrum, ρ(ω,T). Changes observed in ρ(ω,T) are directly reflected on the spectral features of the Raman coupling coefficient, Cαβ(ω). Our data provide evidence for polarization dependence of this coefficient, which has been completely overlooked in studies concerning the experimental determination of Cαβ(ω) through a comparison of neutron and reduced Raman spectra. The current status considering the frequency dependence of the coupling coefficient is briefly reviewed from the theoretical, experimental, and computer simulation points of view. The experimental data suggest that a reconsideration of the approaches employed should be undertaken.

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The central idea of the preceding Comment [J. Chem. Phys. xxx, xxx (2004)] is tackled from different viewpoints and arguments are presented showing its invalidity. First, we show that the presence of non-S8 rings is negligible under the conditions in which our experiment was performed. Then we prove that, even if we consider the non-S8 ring’s presence in the concentrations indicated in the Comment, their contribution to the isotropic Raman intensity is negligible and hence the accuracy of polymer content determination does not change as the authors of the Comment supposed. Finally, we briefly examine the ensuing question of the extent to which quench-and-dissolution methods can give accurate and reproducible results concerning the polymer content in liquid sulfur, demonstrating their inadequacy for reproducible and accurate data. Since reliable ex situ experimental data concerning sulfur’s polymerization do not exist, we vindicate the essence of methodologies that enable the quantification of sulfur’s polymerization from in situ experiments.