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The open-circuit voltage (V

Piezoelectric materials convert between mechanical and electrical energy and are a basis for self-powered electronics. Current piezoelectrics exhibit either large charge (d33) or voltage (g33) coefficients but not both simultaneously, and yet the maximum energy density for energy harvesting is determined by the transduction coefficient: d33*g33. In prior piezoelectrics, an increase in polarization usually accompanies a dramatic rise in the dielectric constant, resulting in trade off between d33 and g33. This recognition led us to a design concept: increase polarization through Jahn-Teller lattice distortion and reduce the dielectric constant using a highly confined 0D molecular architecture. With this in mind, we sought to insert a quasi-spherical cation into a Jahn-Teller distorted lattice, increasing the mechanical response for a large piezoelectric coefficient. We implemented this concept by developing EDABCO-CuCl4 (EDABCO = N-ethyl-1,4-diazoniabicyclo[2.2.2]octonium), a molecular piezoelectric with a d33 of 165 pm/V and g33 of ~2110 × 10−3 V m N−1, one that achieved thusly a combined transduction coefficient of 348 × 10−12 m3 J−1. This enables piezoelectric energy harvesting in EDABCO-CuCl4@PVDF (polyvinylidene fluoride) composite film with a peak power density of 43 µW/cm2 (at 50 kPa), the highest value reported for mechanical energy harvesters based on heavy-metal-free molecular piezoelectric.