Shotgun Crystal Structure Prediction of High-Energy Metastable Materials at Ambient Conditions

ENERGY MATERIAL ADVANCES. 2026.

Wen L., Liu D., Yu T., Мусатова А. М., Kushchuk L., Antanyazov M., Huang Z., Mezentsev I., Kartsev A., Vasenko A., Liu Y.

Metastable materials offer promising properties unattainable in conventional stable structures, yet their intrinsic instability poses a significant obstacle to both theoretical design and experimental synthesis. These challenges largely stem from the lack of a fundamental understanding on such high-energy phases with extraordinary structures, because the efficient exploration of metastable materials remains difficult. To address these issues, here, we develop a shotgun crystal structure prediction (CSP) method to search for high-energy structures rather than focusing solely on the stable ones. Applying this method to allnitrogen materials, we identify a variety of thermodynamically unstable structures ranging from 0D molecules to 3D crystals. Notably, these structures possess a wide range of formation energies, with some cases surpassing the energetic benchmark set by the fully single-bonded cubic gauche nitrogen (cg-N). We demonstrate that the high formation energy arises primarily from the stretched single bonds, and the 0D and 3D structures are more favorable for such distorted configurations, serving as potential candidates of energetic materials. The diversity of the predicted structures implies the effectiveness of this shotgun CSP in discovering exotic configurations. This work not only presents an efficient method for designing high-energy metastable materials at ambient conditions, but also provides crucial insights into the fundamental properties of all-nitrogen compounds.

Keywords: High-energy materials, crystal structure prediction, Metastable materials, Метастабильные материалы, Предсказание кристаллической структуры, Высокоэнергетические материалы

Publication based on the results of: Атомистическое моделирование динамики фотовозбуждённых состояний в новых материалах для солнечной энергетики (2024)