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This paper reports a handy technical scheme to decorate atomic force microscopy (AFM) tips toward tip-enhanced Raman spectroscopy (TERS) applications. The major attraction of these homemade tips lies in that silver decoration can be confined at the apex of commercial tips by the means of an AFM-controlled electrochemical reaction. The reduction of Ag+ occurs in a highly sealed environment to secure the metal coating efficiency. Key factors include silver nitrate solution to provide Ag+, ambient relative humidity and temperature in a humidity cell, electric potential bias, and tip–surface distance. Subsequently, these silver-coated tips are evaluated for TERS measurement of carbon nanotubes (CNTs) so that both morphological and chemical characteristics of CNTs are concurrently obtained. The Raman spectra reveal that our plasmonic tip competently possesses an ∼30-fold local field signal increase and the corresponding TERS image laterally resolves at the single-pixel level.

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