4.8 Article

Reversible Switching between Destructive and Constructive Quantum Interference Using Atomically Precise Chemical Gating of Single-Molecule Junctions

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 25, 页码 9385-9392

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c00928

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资金

  1. National Natural Science Foundation of China [21673195, 21722305, 21703188, U1705254]
  2. National Key R&D Program of China [2017YFA0204902]
  3. China Postdoctoral Science Foundation [2017M622060]
  4. Fundamental Research Funds for the Central Universities [20720200068]
  5. UKRI Future Leaders Fellowship [MR/S015329/2]
  6. Leverhulme Trust Early Career Fellowship [ECF-2018-375]

向作者/读者索取更多资源

This study introduces an atomically precise gating strategy to manipulate the quantum interference patterns at the single-molecule scale, achieving a complete switching from destructive to constructive QI modes and significant conductance modulation at room temperature. The chemical gating effect exerted locally on the pyridine nitrogen through selective interaction with cationic reagents demonstrates unique capabilities in modulating QI and offers potential for developing novel electronic devices.
Quantum interference (QI) plays an imperative role in the operation of molecular devices within the phase-coherent length, and it is vital to harness the patterns of QI, i.e., constructive and destructive interference. However, the size of the single-molecule device is too small compared to most gate electrodes. Those gates act like a backgate to affect the molecular component uniformly. Switching the patterns of QI in the same molecular skeleton remains challenging. Here, we develop the atomically precise gating strategy that manipulates the frontier orbitals of molecular components, achieving the complete switching of QI patterns between destructive to constructive QI and leading to a significant conductance modulation at room temperature. The chemical gating effect is exerted locally on the pyridine nitrogen through the selective interaction to cationic reagents, with which we can also control the switching reversibility as desired. We demonstrate the unique effect of atomically precise gating to modulate the quantum interference at the single-molecule scale, opening an avenue to develop new-conceptual electronic devices.

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