2024
DOI: 10.1021/jacs.3c14079
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Chemistry of the Au–Thiol Interface through the Lens of Single-Molecule Flicker Noise Measurements

Umar Rashid,
William Bro-Jørgensen,
KB Harilal
et al.

Abstract: Chemistry of the Au−S interface at the nanoscale is one of the most complex systems to study, as the nature and strength of the Au−S bond change under different experimental conditions. In this study, using mechanically controlled break junction technique, we probed the conductance and analyzed Flicker noise for several aliphatic and aromatic thiol derivatives and thioethers. We demonstrate that Flicker noise can be used to unambiguously differentiate between stronger chemisorption (Au− SR) and weaker physisor… Show more

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Cited by 8 publications
(2 citation statements)
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“…[12][13][14] The solvent dielectric can also tune the strength of interfacial electric fields shown to catalyze in situ chemical transformations. 15,16 Critically, most non-polar solvents do not exhibit sufficiently low vapor pressures to inhibit significant evaporation at elevated temperatures or over extended periods at RT. 9 To minimize the impact of varying solution concentration, previous studies have measured samples at high temperatures prior to low temperature 5 or have periodically added pure solvent to analyte solutions.…”
mentioning
confidence: 99%
“…[12][13][14] The solvent dielectric can also tune the strength of interfacial electric fields shown to catalyze in situ chemical transformations. 15,16 Critically, most non-polar solvents do not exhibit sufficiently low vapor pressures to inhibit significant evaporation at elevated temperatures or over extended periods at RT. 9 To minimize the impact of varying solution concentration, previous studies have measured samples at high temperatures prior to low temperature 5 or have periodically added pure solvent to analyte solutions.…”
mentioning
confidence: 99%
“…In STM-based break junction (STM-BJ) experiments, solvents comprising heteroatoms with a relatively high binding affinity for gold have been found to influence the energetic level alignment between the dominant conducting orbital(s) of the molecule and the Fermi level ( E F ) of the electrodes, rendering junction tunneling conductance solvent-dependent. One such solvent, 1-bromonaphthalene (BN), can even influence the most probable binding geometry of gold–thiol junctions by competing for undercoordinated surface sites . Should charge hopping processes dominate transport, the solvent environment around the junction may also impact conductance by modulating outer sphere reorganization energies associated with sequential electron transfer events. The solvent dielectric can also tune the strength of interfacial electric fields shown to catalyze in situ chemical transformations. , …”
mentioning
confidence: 99%