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Alignment, functionalization and detection of carbon nanotube (CNT) bundles are vital processes for utilizing this one-dimensional nanomaterial in electronics. Here, we report a polymer-assisted wet shearing method to acquire super-aligned crater-patterned CNT arrays by nanobubble (NB) self-assembly with a "migrate and aggregation" mechanism and use craters to controllably mold even-sized nanodisks periodically along CNT bundles with tunable densities. This green, low-cost method can be extended to diverse substrates and fabricate different nanodisks. As an example, the Ag-nanodisk-patterned CNT arrays are utilized as substrates of surface-enhanced Raman scattering (SERS) for rhodamine 6G (R6G) and methylene blue (MB) in which a linear correlation is found between the SERS intensity and the CNT bundle density due to the periodic distribution of hot spots, enabling a spectral detection of CNT bundles and their densities by conventional dye molecules. Distinguishing from routine morphological characterization, this spectral method possesses an enhanced accuracy and a detection range of 0.1–2 μm–1, showing its uniqueness in the detection of CNT bundle density since the intensity of traditional spectral merely relates to the quantity of CNTs, exhibiting its potential in future CNT-bundle-based electronics.

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