Quantum mechanics studies on the stability mechanism and detonation performance of high-energy-density materials

We developed a couple of quantum mechanics methods specialized for simulating crystal-level high-energy-density materials (HEDMs). Using these methods, we first studied how nitrogen-aromatics are stabilized under various surroundings. We discovered the presence of dual-aromaticity in five-membered systems like pentazole and C-N heterocycles. Later, anions of these dual-aromatics were found to have abnormal reactivity in acidic surroundings due to a competition between their basicity and dual-aromaticity. At lower acidity, basicity overcomes dual-aromaticity and the heterocyclic anions undergo acid-base neutralization. When the acidity becomes sufficiently high, dual-aromaticity defeats basicity. These anions turn to resist protonation and violate acid-base neutralization, earning extra stability and enhanced firmness through intermolecular interactions with surrounding acidic ions. No such anomaly was observed in organic solutions like benzene and THF, and these solvents present little influence on stability of the heterocyclic anions. This acid-trapping strategy, a promising strategy for facilitating nitrogen-aromatics to productive yielding, was found also applicable to five-membered pnictogen heterocycles and square tetranitrogen. Second, we focused on how various physicochemical characteristics of HEDMs affecting their power level and their stability. High-throughput calculations were conducted for hundreds of HEDMs. Based on the statistical analysis of calculated data and the machine-learning techniques, in-crystal interspecies interactions were identified to be the one that provokes the performance stability contradiction of HEDMs. The optimal range of key features for efficient rational design of advanced HEDMs was delivered. Based on proposed guidelines, three new thermostable HEDMs containing bridged, 3,5-dinitropyrazole moieties were successfully synthesized, characterized, and evaluated.