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The NIVO\u2010dsDNA interaction was evaluated, in incubated solutions, by differential pulse voltammetry, UV\u2010Visible spectrophotometry and gel electrophoresis, and <jats:italic>in\u2005situ<\/jats:italic> with dsDNA\u2010, poly[G]\u2010 or poly[A]\u2010electrochemical biosensors, by differential pulse voltammetry, electrochemical impedance spectroscopy, and quartz crystal microbalance. The interfacial behaviour of the dsDNA\u2010electrochemical biosensor was also investigated by cyclic voltammetry and electrochemical impedance spectroscopy. The NIVO\u2010dsDNA interaction mechanism caused, for shorter times, the binding of the NIVO to DNA, resulting in a NIVO\u2010dsDNA complex, and for longer times, the relaxation\/unwinding of this complex structure. 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