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Unimolecular dissociation reactions of small molecules were investigated. The thermal decomposition of N2O was investigated in a detailed way. By using the methods of shock waves and adiabatic compression the reaction was studied between 1200 and 2500K. All experimental results which describe a variation of the low pressure limiting rate of about eleven orders of magnitude, are in good agreement. This example and others were selected for a detailed theoretical analysis of unimolecular reactions of three- and four-atomic molecules. For shock tube experiments up to about 1000 atmospheres, a shock tube with 70 mm internal diameter was constructed and put into operation. Driving pressures up to about 200 atmospheres were used for experiments on N2O- and N2H4- decomposition, which gave data on the high pressure limiting rate of both dissociations.