AbstractThe influence of thermally excited vibrations on vibronic spectra (absorption, CARS excitation profile and resonance background) has been modelled for polyatomic molecules in solution. It is shown that for a model describing some polymethine compounds, the spectra depend only slightly on temperature except in the case of a resonance background and an excitation profile of vibrations with a relatively high value of the origin shift parameter (Δ>1). The investigations of low‐frequency vibrations by resonance CARS to giving information about some molecular parameters is propos