Ambient-Stable Polymeric Nitrogen Achieved through Multi-Stage Computational Design

The four-decade quest for synthesizing ambient-stable polymeric nitrogen, a promising high-energy-density material, remains an unsolved challenge in materials science. We develop a multi-stage computational strategy employing density functional tight-binding-based rapid screening combined with density functional theory refinement and global structure searching, effectively bridging computational efficiency with quantum accuracy. This integrated approach identifies four novel polymeric nitrogen phases (Fddd, P3221, I\bar4m2, and P6522) that are thermodynamically stable at ambient pressure. Remarkably, the helical P6522 configuration demonstrates exceptional thermal resilience up to 1500 K, representing a predicted polymeric nitrogen structure that maintains stability under both atmospheric pressure and high-temperature extremes. Our methodology establishes a paradigm-shifting framework for the accelerated discovery of metastable energetic materials, resolving critical bottlenecks in theoretical predictions while providing experimentally actionable targets for polymeric nitrogen synthesis.