Final published version
Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Selective anchoring groups for molecular electronic junctions with ITO electrodes
AU - Planje, I.J.
AU - Davidson, R.J.
AU - Vezzoli, A.
AU - Daaoub, A.
AU - Sangtarash, S.
AU - Sadeghi, H.
AU - Martín, S.
AU - Cea, P.
AU - Lambert, C.J.
AU - Beeby, A.
AU - Higgins, S.J.
AU - Nichols, R.J.
PY - 2021/2/26
Y1 - 2021/2/26
N2 - Indium tin oxide (ITO) is an attractive substrate for single-molecule electronics since it is transparent while maintaining electrical conductivity. Although it has been used before as a contacting electrode in single-molecule electrical studies, these studies have been limited to the use of carboxylic acid terminal groups for binding molecular wires to the ITO substrates. There is thus the need to investigate other anchoring groups with potential for binding effectively to ITO. With this aim, we have investigated the single-molecule conductance of a series of eight tolane or “tolane-like” molecular wires with a variety of surface binding groups. We first used gold-molecule- gold junctions to identify promising targets for ITO selectivity. We then assessed the propensity and selectivity of carboxylic acid, cyanoacrylic acid, and pyridinium-squarate to bind to ITO and promote the formation of molecular heterojunctions. We found that pyridinium squarate zwitterions display excellent selectivity for binding to ITO over gold surfaces, with contact resistivity comparable to that of carboxylic acids. These single-molecule experiments are complemented by surface chemical characterization with X-ray photoelectron spectroscopy, quartz crystal microbalance, contact angle determination, and nanolithography using an atomic force miscroscope. Finally, we report the first density-functional theory calculations involving ITO electrodes to model charge transport through ITO-molecule-gold heterojunctions.
AB - Indium tin oxide (ITO) is an attractive substrate for single-molecule electronics since it is transparent while maintaining electrical conductivity. Although it has been used before as a contacting electrode in single-molecule electrical studies, these studies have been limited to the use of carboxylic acid terminal groups for binding molecular wires to the ITO substrates. There is thus the need to investigate other anchoring groups with potential for binding effectively to ITO. With this aim, we have investigated the single-molecule conductance of a series of eight tolane or “tolane-like” molecular wires with a variety of surface binding groups. We first used gold-molecule- gold junctions to identify promising targets for ITO selectivity. We then assessed the propensity and selectivity of carboxylic acid, cyanoacrylic acid, and pyridinium-squarate to bind to ITO and promote the formation of molecular heterojunctions. We found that pyridinium squarate zwitterions display excellent selectivity for binding to ITO over gold surfaces, with contact resistivity comparable to that of carboxylic acids. These single-molecule experiments are complemented by surface chemical characterization with X-ray photoelectron spectroscopy, quartz crystal microbalance, contact angle determination, and nanolithography using an atomic force miscroscope. Finally, we report the first density-functional theory calculations involving ITO electrodes to model charge transport through ITO-molecule-gold heterojunctions.
KW - Anchoring groups
KW - Indium tin oxide
KW - ITO
KW - Scanning tunneling microscopy
KW - Single-molecule conductance
KW - STM break junction
KW - STM-I(t)
KW - X-ray photoelectron spectroscopy
KW - Carboxylic acids
KW - Contact angle
KW - Density functional theory
KW - Electrodes
KW - Gold
KW - Heterojunctions
KW - Indium compounds
KW - Molecules
KW - Nanowires
KW - Tin oxides
KW - X ray photoelectron spectroscopy
KW - Contact angle determination
KW - Contact resistivities
KW - Electrical conductivity
KW - Electrical studies
KW - Molecular electronic junction
KW - Single molecule conductance
KW - Single molecule experiments
KW - Single-molecule electronics
KW - Substrates
U2 - 10.1021/acssensors.0c02205
DO - 10.1021/acssensors.0c02205
M3 - Journal article
VL - 6
SP - 530
EP - 537
JO - ACS Sensors
JF - ACS Sensors
SN - 2379-3694
IS - 2
ER -