Single-Molecule Reaction Chemistry in Patterned Nanowells

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• 作者：Delphine Bouilly ; Jason Hon ; Nathan S. Daly ; Scott Trocchia ; Sefi Vernick ; Jaeeun Yu ; Steven Warren ; Ying Wu ; Ruben L. Gonzalez Jr. ; Kenneth L. Shepard ; Colin Nuckolls
• 刊名：Nano Letters
• 出版年：2016
• 出版时间：July 13, 2016
• 年：2016
• 卷：16
• 期：7
• 页码：4679-4685
• 全文大小：534K
• 年卷期：0
• ISSN：1530-6992

文摘

A new approach to synthetic chemistry is performed in ultraminiaturized, nanofabricated reaction chambers. Using lithographically defined nanowells, we achieve single-point covalent chemistry on hundreds of individual carbon nanotube transistors, providing robust statistics and unprecedented spatial resolution in adduct position. Each device acts as a sensor to detect, in real-time and through quantized changes in conductance, single-point functionalization of the nanotube as well as consecutive chemical reactions, molecular interactions, and molecular conformational changes occurring on the resulting single-molecule probe. In particular, we use a set of sequential bioconjugation reactions to tether a single-strand of DNA to the device and record its repeated, reversible folding into a G-quadruplex structure. The stable covalent tether allows us to measure the same molecule in different solutions, revealing the characteristic increased stability of the G-quadruplex structure in the presence of potassium ions (K⁺) versus sodium ions (Na⁺). Nanowell-confined reaction chemistry on carbon nanotube devices offers a versatile method to isolate and monitor individual molecules during successive chemical reactions over an extended period of time.