Physics-informed data-driven topology-supported precursor screening strategy for designing all-organic polyimide dielectrics with deep traps and wide-temperature-range

Data-driven screening identifies melamine as optimal precursor for QbPIs. • Star-shaped topology expands HOMO-LUMO gap, introduces deep traps, and stabilizes Ag/dielectric interface. • Topological structure suppresses conduction loss and charge injection, disrupting charge-transport pathways. • QbPI-1.75 achieves 5.39 J/cm 3 at 25 °Cand 3.29 J/cm 3 at 200 °C with high efficiency. • Scalable, cost-effective design provides a platform for high-temperature polymer dielectrics beyond polyimides. The development of high-power electronics demands polymer dielectrics with high thermal stability and dielectric performance. However, most materials suffer performance degradation in harsh environments due to increased electrical conductivity. Herein, a physics-informed data-driven topology-supported precursor screening strategy was proposed to design quasi-branched polyimides (QbPIs) with enhanced energy density ( U e ) and charge-discharge efficiency ( η ) at elevated temperatures. By constructing automated screening workflow, key descriptors involving HOMO-LUMO gap ( Gap ) and dielectric constant ( ε r ) were sufficiently evaluated to form multi-parameter ranking framework, in which melamine was identified as the optimal topological center for constructing QbPIs with tunable topological ratios (0–2.5%). Notably, the resulting star-shaped topological structure effectively regulates charge transport and dielectric behavior through a cooperative mechanism. It increases the Gap , introduces deep-level traps, and stabilizes the Ag/dielectric interface, which together suppress conduction loss and charge injection, effectively disrupting long-range charge-transport pathways. The optimized QbPI-1.75 exhibited outstanding capacitive performance, delivering 5.39 J cm −3 ( U e ) with 94% ( η ) at 25 °C, and retaining 3.29 J cm −3 with 78.41% at 200 °C, far exceeding that of pure PI (1.35 J cm −3 , 87.6% η at 25 °C). This work establishes a fundamental structure-property relationship for topological PIs and provides a facile design strategy applicable to other high-temperature polymer dielectrics. A Physics-Informed Data-Driven Topology-Supported Precursor Screening Strategy screens melamine as the optimal precursor to construct star -shaped all-organic polyimide dielectric films. At 25 °C/200 °C, QbPI-1.75 exhibited breakdown strength 51.58%/32.61% higher than PI and energy densities of 5.39/3.29 J cm −3 , respectively. The star topology enhanced planar stacking to suppress thermal motion, introduced deep traps, and broadened the bandgap, synergistically blocking charge transport and raising the excitation barrier, thus overcoming material bottlenecks for high-temperature capacitive energy storage. This scalable, cost-effective approach is extendable to other polymer systems. Download: Download high-res image (107KB) Download: Download full-size image