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The algebra of primary cohomology operations computed by the well-known Steenrod algebra is one of the most powerful tools of algebraic topology. This book computes the algebra of secondary cohomology operations which enriches the structure of the Steenrod algebra in a new and unexpected way.The book solves a long-standing problem on the algebra of secondary cohomology operations by developing a new algebraic theory of such operations. The results have strong impact on the Adams spectral sequence and hence on the computation of homotopy groups of spheres.