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Periodic structures in chemical kinetic systems can be evaluated by an extension of the well-known method of harmonic balance, which yields very simple expressions in the case of linear systems containing only zero and first order reactions. The far more interesting non-linear systems containing e.g. second order reactions which in case of open systems far from thermodynamic equilibrium give rise to non-classical phenomena like oscillations, chemical waves, excitability, hysteresis, multistability, dissipative structures etc. can be treated in a similar way by introducing new pseudo-linear quantities utilizing certain group properties of harmonic expansions. The resulting complicated implicit non-linear algebraic equations are solved by a method developed by Powell and show good convergence. Since this method - in contrast to the conventional method of simulation - is independent from the stability of the periodic structure to be evaluated it can even be applied to unstable cases where the simulation method necessarily fails. An evaluation of the stability is included in the developed computer program.

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Unrestricted Harmonic Balance: A General Method to Evaluate Periodic Structures in Time and/or Space of Arbitrary Stability for Non-linear Chemical Reaction and Reaction-Diffusion Systems.I. Theory and Computer Program for Time-dependent Systems