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Nanometer thin single-walled carbon nanotube (CNT) films collected from theaerosol chemical deposition reactors have gathered attention for theirpromising applications. Densification of these pristine films provides animportant way to manipulate the mechanical, electronic, and optical properties.To elucidate the underlying microstructural level restructuring, which isultimately responsible for the change in properties, we perform large scalevector-based mesoscopic distinct element method simulations in conjunction withelectron microscopy and spectroscopic ellipsometry characterization of pristineand densified films by drop-cast volatile liquid processing. Matching themicroscopy observations, pristine CNT films with finite thickness are modeledas self-assembled CNT networks comprising entangled dendritic bundles withbranches extending down to individual CNTs. Simulations of the film underuniaxial compression uncover an ultra-soft densification regime extending to a~75% strain, which is likely accessible with the surface tensional forcesarising from liquid surface tension during the evaporation. When removing theloads, the pre-compressed samples evolve into homogeneously densified filmswith thickness values depending on both the pre-compression level and thesample microstructure. The significant reduction in thickness, confirmed by ourspectroscopic ellipsometry, is attributed to the underlying structural changesoccurring at the 100 nm scale, including the zipping of the thinnest dendriticbranches.

Densification of Single-Walled Carbon Nanotube Films: Mesoscopic Distinct Element Method Simulations and Experimental Validation