Comprehensive theoretical study of the correlation between the energetic and thermal stabilities for the entire set of 1812 C60 isomers

• Published in: Journal of applied physics 2022-08, Vol.132 (6)
• Main Authors: Aghajamali, Alireza, Karton, Amir
• Format: Article
• Language: English
• Subjects: Applied physics; Buckminsterfullerene; Energy distribution; Fragmentation; Fullerenes; Isomerization; Isomers; Machine learning; Molecular dynamics; Simulation; Statistical correlation; Temperature; Thermal stability; Thermodynamic properties
• ISSN: 0021-8979; 1089-7550
• DOI: 10.1063/5.0100612

The thermal stability of fullerenes plays a fundamental role in their synthesis and in their thermodynamic and kinetic properties. Here, we perform extensive molecular dynamics (MD) simulations using an accurate machine-learning-based Gaussian Approximation Potential (GAP-20) force field to investigate the energetic and thermal properties of the entire set of 1812 C 60 isomers. Our MD simulations predict a comprehensive and quantitative correlation between the relative isomerization energy distribution of the C 60 isomers and their thermal fragmentation temperatures. We find that the 1812 C 60 isomers span over an energetic range of over 400 kcal mol − 1, where the majority of isomers ( ∼85%) lie in the range between 90 and 210 kcal mol − 1 above the most stable C 60- I h buckminsterfullerene. Notably, the MD simulations show a clear statistical correlation between the relative energies of the C 60 isomers and their fragmentation temperature. The maximum fragmentation temperature is 4800 K for the C 60- I h isomer and 3700 K for the energetically least stable isomer, where nearly 80% of isomers lie in a temperature window of 4000–4500 K. In addition, an Arrhenius-based approach is used to map the timescale gap between simulation and experiment and establish a connection between the MD simulations and fragmentation temperatures.