Car‐Parrinello Molecular Dynamics Elucidate Atomic Nitrogen Reactivity Under Nanoflask (C70) Confinement Conditions

Abstract We performed an ab initio molecular dynamics study with a nitrogen atom in the 1/2 spin state, which corresponds to an excited electronic state, in contrast to the ground state with 3/2 spin state. This N atom was encapsulated with an H 2 molecule in a C70 fullerene, as a “nanoflask” for experimentation. This approach was initially proposed by Morinaka and colleagues (Angew. Chem. Int. Ed. 2017, 56, 6488–6491), where they demonstrated, using spectroscopy, that the N( 4 S ) atom, does not react with the H 2 molecule. By analyzing the trajectory from Car‐Parrinello molecular dynamics simulations and performing Density Functional Theory, Quantum Theory of Atoms in Molecules, Reduced Density Gradient and Interaction Region Indicator calculations, we successfully reproduced the experiment observations, examining the interaction between the N atom and the H 2 molecule encapsulated within the fullerene C 70 .