We used covalent attachments to single-walled carbon nanotubes (SWNTs) to fabricate singlemolecule
electronic devices. The technique does not rely on submicrometer lithography or precision
mechanical manipulation, but instead uses circuit conductance to monitor and control covalent
attachment to an electrically connected SWNT. Discrete changes in the circuit conductance revealed
chemical processes happening in real time and allowed the SWNT sidewalls to be deterministically
broken, reformed, and conjugated to target species. By control领 the chemistry through
electronically controlled electrochemical potentials, we were able to achieve single chemical
attachments. We routinely functionalized pristine, defect-free SWNTs at one, two, or more sites and
demonstrated three-terminal devices in which a single attachment controls the electronic response.
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