Multiscale modeling strategy to solve fullerene formation mystery

TL;DR

This paper reviews atomistic mechanisms of fullerene formation and proposes a multiscale modeling strategy combining graph theory, molecular dynamics, and ab initio calculations to understand isomer selection.

Contribution

It introduces a comprehensive multiscale modeling approach integrating various techniques to investigate fullerene isomer formation mechanisms.

Findings

Atomic-scale processes influence fullerene isomer abundance.

No conclusive evidence favors a specific atomistic mechanism.

Proposed strategy combines graph theory, molecular dynamics, and ab initio methods.

Abstract

Since fullerene formation occurs under conditions where direct observation of atomic-scale reactions is not possible, modeling is the only way to reveal atomistic mechanisms which can lead to selection of abundant fullerene isomers (like C60-Ih). In the present paper we review the results obtained for different atomistic mechanisms by various modeling techniques. Although it seems that atomic-scale processes related to odd fullerenes (such as growth by consecutive insertions of single carbon atoms and rearrangements of the sp$^2$ structure promoted by extra sp atoms) provide the main contribution to selection of abundant isomers, at the moment there is no conclusive evidence in favor of any particular atomistic mechanism. Thus, the following multiscale modeling strategy to solve the mystery of the high yield of abundant fullerene isomers is suggested. On the one hand, sets of reactions between fullerene isomers can be described using theoretical graph techniques. On the other hand, reaction schemes can be revealed by classical molecular dynamics simulations with subsequent refinement of the activation barriers by ab initio calculations. Based on the reaction sets with the reaction probabilities derived in this way, the different atomistic mechanisms of abundant fullerene isomer selection can be compared by kinetic models.