Byers, Joshua C., Paulose Nadappuram, Binoy, Perry, David, McKelvey, Kim, Colburn, Alex W. and Unwin, Patrick R. (2015) Single molecule electrochemical detection in aqueous solutions and ionic liquids. Analytical Chemistry, 87 (20). pp. 10450-10456. doi:10.1021/acs.analchem.5b02569 ISSN 0003-2700.

PDF WRAP_1050272-ch-290915-unwin_main_single_molecule (1).pdf - Accepted Version Embargoed item. Restricted access to Repository staff only - Requires a PDF viewer. Download (781Kb)

Request Changes to record.

Abstract

Single molecule electrochemical detection (SMED) is an extremely challenging aspect of electroanalytical chemistry, requiring unconventional electrochemical cells and measurements. Here, SMED is reported using a ‘quad-probe’ (4-channel probe) pipet cell, fabricated by depositing carbon pyrolytically into two diagonally opposite barrels of a laser-pulled quartz quadruple-barreled pipet and filling the open channels with electrolyte solution, and quasi-reference counter electrodes. A meniscus forms at the end of the probe covering the two working electrodes, and is brought into contact with a substrate working electrode surface. In this way, a nanogap cell is produced whereby the two carbon electrodes in the pipet can be used to promote redox cycling of an individual molecule with the substrate. Anti-correlated currents generated at the substrate and tip electrodes, at particular distances (typically 10’s of nanometers) are consistent with the detection of single molecules. The low background noise realized in this droplet format opens up new opportunities in single molecule electrochemistry, including the use of ionic liquids, as well as aqueous solution, and the quantitative assessment and analysis of factors influencing redox cycling currents, due to a precisely known gap size.

Item Type:	Journal Article
Divisions:	Faculty of Science, Engineering and Medicine > Science > Chemistry
Journal or Publication Title:	Analytical Chemistry
Publisher:	American Chemical Society
ISSN:	0003-2700
Official Date:	23 September 2015
Dates:	Date Event 23 September 2015 Published 23 September 2015 Accepted 8 July 2015 Submitted
Volume:	87
Number:	20
Page Range:	pp. 10450-10456
DOI:	10.1021/acs.analchem.5b02569
Status:	Peer Reviewed
Publication Status:	Published
Access rights to Published version:	Restricted or Subscription Access
Date of first compliant deposit:	22 December 2015

Request changes or add full text files to a record

Repository staff actions (login required)

View Item