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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 - Single-Molecule Conductance Behavior of Molecular Bundles
AU - Bara-Estaún, Alejandro
AU - Planje, Inco J.
AU - Almughathawi, Renad
AU - Naghibi, Saman
AU - Vezzoli, Andrea
AU - Milan, David C.
AU - Lambert, Colin
AU - Martin, Santiago
AU - Cea, Pilar
AU - Nichols, Richard J.
AU - Higgins, Simon J.
AU - Yufit, Dmitry S.
AU - Sangtarash, Sara
AU - Davidson, Ross J.
AU - Beeby, Andrew
PY - 2023/12/25
Y1 - 2023/12/25
N2 - Controlling the orientation of complex molecules in molecular junctions is crucial to their development into functional devices. To date, this has been achieved through the use of multipodal compounds (i.e., containing more than two anchoring groups), resulting in the formation of tri/tetrapodal compounds. While such compounds have greatly improved orientation control, this comes at the cost of lower surface coverage. In this study, we examine an alternative approach for generating multimodal compounds by binding multiple independent molecular wires together through metal coordination to form a molecular bundle. This was achieved by coordinating iron(II) and cobalt(II) to 5,5′-bis(methylthio)-2,2′-bipyridine (L 1 ) and (methylenebis(4,1-phenylene))bis(1-(5-(methylthio)pyridin-2-yl)methanimine) (L 2 ) to give two monometallic complexes, Fe-1 and Co-1, and two bimetallic helicates, Fe-2 and Co-2. Using XPS, all of the complexes were shown to bind to a gold surface in a fac fashion through three thiomethyl groups. Using single-molecule conductance and DFT calculations, each of the ligands was shown to conduct as an independent wire with no impact from the rest of the complex. These results suggest that this is a useful approach for controlling the geometry of junction formation without altering the conductance behavior of the individual molecular wires.
AB - Controlling the orientation of complex molecules in molecular junctions is crucial to their development into functional devices. To date, this has been achieved through the use of multipodal compounds (i.e., containing more than two anchoring groups), resulting in the formation of tri/tetrapodal compounds. While such compounds have greatly improved orientation control, this comes at the cost of lower surface coverage. In this study, we examine an alternative approach for generating multimodal compounds by binding multiple independent molecular wires together through metal coordination to form a molecular bundle. This was achieved by coordinating iron(II) and cobalt(II) to 5,5′-bis(methylthio)-2,2′-bipyridine (L 1 ) and (methylenebis(4,1-phenylene))bis(1-(5-(methylthio)pyridin-2-yl)methanimine) (L 2 ) to give two monometallic complexes, Fe-1 and Co-1, and two bimetallic helicates, Fe-2 and Co-2. Using XPS, all of the complexes were shown to bind to a gold surface in a fac fashion through three thiomethyl groups. Using single-molecule conductance and DFT calculations, each of the ligands was shown to conduct as an independent wire with no impact from the rest of the complex. These results suggest that this is a useful approach for controlling the geometry of junction formation without altering the conductance behavior of the individual molecular wires.
KW - Inorganic Chemistry
KW - Physical and Theoretical Chemistry
U2 - 10.1021/acs.inorgchem.3c01943
DO - 10.1021/acs.inorgchem.3c01943
M3 - Journal article
VL - 62
SP - 20940
EP - 20947
JO - Inorganic Chemistry
JF - Inorganic Chemistry
SN - 0020-1669
IS - 51
ER -