Preferred Synthesis of Armchair Transition Metal Dichalcogenide Nanotubes

Abstract

In this work, we present the synthesis of transition-metal dichalcogenide (TMDC) nanotubes with a preferred chiral angle. SnS2, MoS2, and WS2 are formed with high yield and structural purity inside the channels of boron nitride nanotubes. Atomic-resolution imaging, nano-area electron diffraction, and Circular Dichroism spectroscopy reveal that these synthesized TMDC nanotubes prefer to have an armchair configuration, with a probability up to 84%. Density functional theory reveals a negligible difference in the formation energy between armchair and zigzag nanotubes, suggesting that the chirality preference does not originate from the differences in structural stability. However, a detailed TEM investigation revealed that these TMDC nanotubes formed via a transition state of nanoribbons, and these nanoribbons are energetically more stable in a zigzag configuration. Subsequent machine learning potential molecular dynamics simulations verify that zigzag nanoribbons do roll up to form an armchair SnS2 nanotubes. Finally, this "zigzag nanoribbon to armchair nanotube" transition process is directly observed in real time by in-situ transmission electron microscopy. This work demonstrates the first, but likely general, experimental strategy for synthesizing chirality-preferred TMDC nanotubes.