Novel High-Entropy Polymers with Superior Capacitive Energy Storage

• • Configurational entropy threshold: ΔS_conf ≥ 1.5R is required for a high-entropy state in polymers, necessitating at least five distinct chemical bond types with controlled molar fractions; this criterion mirrors the established definition for alloys and ceramics, providing a quantitative design rule for entropy-stabilized polymers. • • Proton irradiation enables high-entropy polymer synthesis: Low-dose proton irradiation induces multiple chemical bonds, as evidenced by AFM-IR spectroscopy and phase-field simulations, achieving the required ΔS_conf without compromising polymer integrity; this technique offers a scalable route for industrial production of high-entropy polymers. • • Enhanced capacitive energy storage: High-entropy polymers exhibit reduced ferroelectric loss and improved discharged energy density (U_d) and charge/discharge efficiency (η) compared to pristine relaxor ferroelectric polymers; these improvements directly address the bottleneck of high losses in dielectric capacitors for pulsed power applications. • • Phase-field simulation validation: Simulations incorporating random field variance (σ = 88 MV m⁻¹) and diffused Curie temperature (Δ = 3.6 K) reproduce experimental polarization-electric field loops, confirming that the high-entropy state stabilizes the relaxor behavior and suppresses hysteresis; this predictive capability accelerates future material optimization.