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As it is known, in living cells the genetic information is encoded by molecule of deoxyribonucleic acid – DNA. DNA is one of the two types of nucleic acids providing storage, transmission from generation to generation, and realization of genetic program of development and functioning of living organisms. Therefore, now molecular computations using DNA strands are developed very actively. This study is devoted to application of the method of Raman spectroscopy for increasing reliability of molecular computations using DNA strands – namely, for express and remote control and measurement of parameters of media, where biochemical reactions with DNA molecules occur. The results of the elaborated method of identification and determination of concentration of individual nitrogenous bases and of the total concentration of DNA in solutions by Raman spectra are presented. Application of artificial neural networks provided successful solution of the specified inverse problem. It has been demonstrated that the method of Raman spectroscopy with the help of artificial neural networks allows one to determine type and concentration of nitrogenous bases (adenine, cytosine, guanine) using their specific spectral markers, with the accuracy of determination of concentration not worse than 0.02-0.03 g/l.