Title | Complex formation dynamics in a single-molecule electronic device |
Authors | Wen, Huimin Li, Wengang Chen, Jiewei He, Gen Li, Longhua Olson, Mark A. Sue, Andrew C.H. Stoddart, J. Fraser Guo, Xuefeng |
Affiliation | Peking Univ, Coll Chem & Mol Engn, State Key Lab Struct Chem Unstable & Stable Speci, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China. Tianjin Univ, Sch Pharmaceut Sci & Technol, Inst Mol Design & Synth, Tianjin 300072, Peoples R China. Jiangsu Univ, Sci Res Acad, Zhenjiang 212013, Peoples R China. Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA. Peking Univ, Coll Engn, Dept Mat Sci & Engn, Beijing 100871, Peoples R China. Peking Univ, Coll Chem & Mol Engn, State Key Lab Struct Chem Unstable & Stable Speci, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China. Sue, ACH Stoddart, JF (reprint author), Tianjin Univ, Sch Pharmaceut Sci & Technol, Inst Mol Design & Synth, Tianjin 300072, Peoples R China. Sue, ACH Stoddart, JF (reprint author), Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA. Guo, XF (reprint author), Peking Univ, Coll Engn, Dept Mat Sci & Engn, Beijing 100871, Peoples R China. |
Keywords | WALLED CARBON NANOTUBES ON-WIRE LITHOGRAPHY ELECTRICAL DETECTION JUNCTIONS TRANSPORT SPECTROSCOPY RECOGNITION CONDUCTANCE KINETICS DNA |
Issue Date | 2016 |
Publisher | SCIENCE ADVANCES |
Citation | SCIENCE ADVANCES.2016,2(11). |
Abstract | Single-molecule electronic devices offer unique opportunities to investigate the properties of individual molecules that are not accessible in conventional ensemble experiments. However, these investigations remain challenging because they require (i) highly precise device fabrication to incorporate single molecules and (ii) sufficient time resolution to be able to make fast molecular dynamic measurements. We demonstrate a graphene-molecule single-molecule junction that is capable of probing the thermodynamic and kinetic parameters of a host-guest complex. By covalently integrating a conjugated molecular wire with a pendent crown ether into graphene point contacts, we can transduce the physical [2]pseudorotaxane (de)formation processes between the electron-rich crown ether and a dicationic guest into real-time electrical signals. The conductance of the single-molecule junction reveals two-level fluctuations that are highly dependent on temperature and solvent environments, affording a non-destructive means of quantitatively determining the binding and rate constants, as well as the activation energies, for host-guest complexes. The thermodynamic processes reveal the host-guest binding to be enthalpy-driven and are consistent with conventional H-1 nuclear magnetic resonance titration experiments. This electronic device opens up a new route to developing single-molecule dynamics investigations with microsecond resolution for a broad range of chemical and biochemical applications. |
URI | http://hdl.handle.net/20.500.11897/476580 |
ISSN | 2375-2548 |
DOI | 10.1126/sciadv.1601113 |
Indexed | SCI(E) |
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