The Conductance and Thermopower Behavior of Pendent Trans-Coordinated Palladium(II) Complexes in Single-Molecule Junctions

Bastante, P. and Davidson, R.J. and Al Malki, W. and Salthouse, R.J. and Cea, P. and Martin, S. and Batsanov, A.S. and Lambert, C.J. and Bryce, M.R. and Agrait, N. (2024) The Conductance and Thermopower Behavior of Pendent Trans-Coordinated Palladium(II) Complexes in Single-Molecule Junctions. ACS Omega, 9 (36). pp. 38303-38312. ISSN 2470-1343

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Abstract

The present work provides insight into the effect of connectivity within isomeric 1,2-bis(2-pyridylethynyl)benzene (bpb) palladium complexes on their electron transmission properties within gold|single-molecule|gold junctions. The ligands 2,2′-((4,5-bis(hexyloxy)-1,2-phenylene)bis(ethyne-2,1-diyl))bis(4-(methylthio)pyridine) (Lm) and 6,6′-((4,5-bis(hexyloxy)-1,2-phenylene)bis(ethyne-2,1-diyl))bis(3-(methylthio)pyridine) (Lp) were synthesized and coordinated with PdCl2 to give the trans-Pd(Lm or p)Cl2 complexes. X-ray photoelectron spectroscopy (XPS) measurements shed light on the contacting modes of the molecules in the junctions. A combination of scanning tunneling microscopy–break junction (STM–BJ) measurements and density functional theory (DFT) calculations demonstrate that the typical lower conductance of meta- compared with para-connected isomers in a molecular junction was suppressed upon metal coordination. Simultaneously there was a modest increase in both conductance and Seebeck coefficient due to the contraction of the HOMO–LUMO gap upon metal coordination. It is shown that the low Seebeck coefficient is primarily a consequence of how the resonances shift relative to the Fermi energy.

Item Type:
Journal Article
Journal or Publication Title:
ACS Omega
Additional Information:
Export Date: 5 September 2024
ID Code:
223727
Deposited By:
Deposited On:
09 Sep 2024 13:40
Refereed?:
Yes
Published?:
Published
Last Modified:
26 Sep 2024 15:36