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Abstract Microcantilever probes for tip‐enhanced Raman spectroscopy （TERS） have a grainy metal coating that may exhibit multiple plasmon hotspots near the tip apex, which may compromise spatial resolution and introduce imaging artefacts. It is also possible that the optical hotspot may not occur at the mechanical apex, which introduces an offset between TERS and atomic force microscope maps. In this article, a gold nanocone TERS probe is designed and fabricated for 638 nm excitation. The imaging performance is compared to grainy probes by analysing high‐resolution TERS cross‐sections of single‐walled carbon nanotubes. Compared to the tested conventional TERS probes, the nanocone probe exhibited a narrow spot diameter, comparable optical contrast, artefact‐free images, and collocation of TERS and atomic force microscope topographic maps. The 1/ e 2 spot diameter was 12.5 nm and 19 nm with 638 nm and 785 nm excitation, respectively. These results were acquired using a single gold nanocone probe to experimentally confirm feasibility. Future work will include automating the fabrication process and statistical analysis of many probes.
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