期刊
NANO LETTERS
卷 21, 期 19, 页码 8340-8347出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c02915
关键词
molecular electronics; resonant transport; scanning tunneling microscope break-junction (STM-BJ)
类别
资金
- Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences
- U.S. Department of Defense by a MURI (Multi-University Research Initiative) through the Army Research Office (ARO) [W911NF-16-10372]
- Defense Advanced Research Projects Agency [HR00111920027]
This study demonstrates that molecular junctions undergo a reversible transition from nonresonant tunneling to resonant transport as a function of applied bias, which is related to the molecular frontier orbital energies and electrode Fermi levels. Through transient bias-switching experiments, the reversible nature of this transition is revealed.
Efficient long-range charge transport is required for high-performance molecular electronic devices. Resonant transport is thought to occur in single molecule junctions when molecular frontier orbital energy levels align with electrode Fermi levels, thereby enabling efficient transport without molecular or environmental relaxation. Despite recent progress, we lack a systematic understanding of the transition between nonresonant and resonant transport for molecular junctions with different chemical compositions. In this work, we show that molecular junctions undergo a reversible transition from nonresonant tunneling to resonant transport as a function of applied bias. Transient bias-switching experiments show that the nonresonant to resonant transition is reversible with the applied bias. We determine a general quantitative relationship that describes the transition voltage as a function of the molecular frontier orbital energies and electrode Fermi levels. Overall, this work highlights the importance of frontier orbital energy alignment in achieving efficient charge transport in molecular devices.
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