The previous work on the Raman effect in barytes has been briefly reviewed. The Raman effect in natural crystals of barytes has been studied in detail using the 2536.5 λ mercury resonance radiation as exciter. The recorded spectrum consists of not less than 39 Raman lines nearly half of which have been recorded for the first time. Of these 20 lines belong to the first order Raman spectrum and are distributed as follows:-9 lattice lines and 11 lines due to the internal oscillations of the SO4 ion. The frequency shifts of these lines have been accurately measured. The appearance of 11 Raman lines in the first order spectrum of the SO4 ion has been satisfactorily explained on the basis of the lower order of sym...