Abstract

The use of single-molecule junctions for various functions constitutes a central goal of molecular electronics. The functional features and the efficiency of electron transport are dictated by the degree of energy-level alignment (ELA), that is, the offset potential between the electrode Fermi level and the frontier molecular orbitals. Examples manifesting ELA are rare owing to experimental challenges and the large energy barriers of typical model compounds. In this work, single-molecule junctions of organometallic compounds with five metal centers joined in a collinear fashion were analyzed. The single-molecule i-V scans could be conducted in a reliable manner, and the EFMO levels were electrochemically accessible. When the electrode Fermi level (EF ) is close to the frontier orbitals (EFMO ) of the bridging molecule, larger conductance was observed. The smaller |EF -EFMO | gap was also derived quantitatively, unambiguously confirming the ELA. The mechanism is described in terms of a two-level model involving co-tunneling and sequential tunneling processes.

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