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Asymmetric piezoelectric composites exhibit coupling between their macroscopic linear momentum and electric field, a coupling that does not appear at the microscopic scale. This electromomentum coupling constitutes an additional knob to tailor the dynamic response of the medium, analogously to the Willis coupling in elastic composites. Here, we employ topology- and free material optimization approaches to maximize the electromomentum coupling of periodic piezoelectric laminates in the low frequency, long-wavelength limit. We find that the coupling can be enhanced by orders of magnitude, depending on the degrees of freedom in the optimization process. The optimal compositions that we find provide guidelines for the design of metamaterials with maximum electromomentum coupling, paving the way for their integration in wave control applications.