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

Abstract

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[Formula: see text] isomers. Our MD simulations predict a comprehensive and quantitative correlation between the relative isomerization energy distribution of the C[Formula: see text] isomers and their thermal fragmentation temperatures. We find that the 1812 C[Formula: see text] isomers span over an energetic range of over 400 kcal mol[Formula: see text], where the majority of isomers ([Formula: see text]85%) lie in the range between 90 and 210 kcal mol[Formula: see text] above the most stable C[Formula: see text]-[Formula: see text] buckminsterfullerene. Notably, the MD simulations show a clear statistical correlation between the relative energies of the C[Formula: see text] isomers and their fragmentation temperature. The maximum fragmentation temperature is 4800 K for the C[Formula: see text]-[Formula: see text] 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.