Dynamics of growing carbon nanotube interfaces probed by machine learningenabled molecular simulations
Résumé
Carbon nanotubes (CNTs), hollow cylinders of carbon, hold great promise for
advanced technologies, provided their structure remains uniform throughout
their length. Their growth takes place at high temperatures across a tubecatalyst
interface. Structural defects formed during growth alter CNT properties.
These defects are believed to form and heal at the tube-catalyst interface
but an understanding of these mechanisms at the atomic-level is lacking.
Here we present DeepCNT-22, a machine learning force field (MLFF) to drive
molecular dynamics simulations through which we unveil the mechanisms of
CNT formation, from nucleation to growth including defect formation and
healing. We find the tube-catalyst interface to be highly dynamic, with large
fluctuations in the chiral structure of the CNT-edge. This does not support
continuous spiral growth as a general mechanism, instead, at these growth
conditions, the growing tube edge exhibits significant configurational entropy.
We demonstrate that defects form stochastically at the tube-catalyst interface,
but under low growth rates and high temperatures, these heal before
becoming incorporated in the tube wall, allowing CNTs to grow defect-free to
seemingly unlimited lengths. These insights, not readily available through
experiments, demonstrate the remarkable power of MLFF-driven simulations
and fill long-standing gaps in our understanding of CNT growth mechanisms
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Hedman_et_al-2024-Nature_Communications.pdf (3.61 Mo)
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raty-et-al-2024-tailoring-chemical-bonds-to-design-unconventional-glasses.pdf (1.98 Mo)
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