High‑Tc Single-Component Organosilicon Ferroelectric Crystal Obtained by H/F Substitution

Organic single-component ferroelectrics are highly desirable for their low molecular mass, light weight, low processing temperature, and excellent film-forming properties. Organosilicon materials with a strong film-forming ability, weather resistance, nontoxicity, odorlessness, and physiological inertia are very suitable for device applications related to the human body. However, the discovery of high-Tc organic single-component ferroelectrics has been very scarce, and the organosilicon ones even less so. Here, we used a chemical design strategy of H/F substitution to successfully synthesize a single-component organosilicon ferroelectric tetrakis(4-fluorophenylethynyl)silane (TFPES). Systematic characterizations and theory calculations revealed that, compared with the parent nonferroelectric tetrakis(phenylethynyl)silane, fluorination caused slight modifications of the lattice environment and intermolecular interactions, inducing a 4/mmmFmm2-type ferroelectric phase transition at a high Tc of 475 K in TFPES. To our knowledge, this Tc should be the highest among the reported organic single-component ferroelectrics, providing a wide operating temperature range for ferroelectrics. Moreover, fluorination also brought about a significant improvement in the piezoelectric performance. Combined with excellent film properties, the discovery of TFPES provides an efficient path for designing ferroelectrics suitable for biomedical and flexible electronic devices.