We consider the question of fundamental limitations on the performance of eddy-viscosity closure models for turbulent flows, focusing on the Leith model for 2D Large-Eddy Simulation. Optimal eddy viscosities depending on the magnitude of the vorticity gradient are determined subject to minimum assumptions by solving PDE-constrained optimization problems defined such that the corresponding optimal Large-Eddy Simulation best matches the Direct Numerical Simulation. The main finding is that with a fixed cutoff wavenumber $k_c$, the performance of the Large-Eddy Simulation systematically improves as the regularization in the solution of the optimization problem is reduced and this is achieved with the optimal eddy viscosities exhibiting increasingly irregular behavior with rapid oscillations. Since the optimal eddy viscosities do not converge to a well-defined limit as the regularization vanishes, we conclude that the problem of finding an optimal eddy viscosity is not in fact well posed.
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