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Protonation tuning of quantum interference in azulene-type single-molecule junctions
Guogang Yang1, Sara Sangtarash2, Zitong Liu3
1State Key Laboratory of Physical Chemistry of Solid Surfaces , iChEM , Department of Chemical and Biochemical Engineering , College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , China .
Protonation significantly boosts conductance in azulene molecular junctions, especially for molecules with destructive quantum interference. This study reveals how protonation alleviates interference, enhancing electrical conductivity.
Area of Science:
- Molecular electronics
- Quantum chemistry
- Condensed matter physics
Background:
- Single-molecule junctions are crucial for molecular electronics.
- Quantum interference effects significantly influence charge transport in molecules.
- Understanding molecular structure-property relationships is key to designing conductive materials.
Purpose of the Study:
- To investigate the impact of protonation on the conductance of azulene derivatives.
- To explore the role of quantum interference in protonated molecular junctions.
- To correlate experimental conductance changes with theoretical predictions.
Main Methods:
- Synthesis of three azulene derivatives with varying connectivities.
- Conductance measurements of single-molecule junctions.
- Protonation of azulene derivatives using trifluoroacetic acid.
- Theoretical modeling using a parameter-free theory of connectivity.
Main Results:
- Protonated azulene molecular junctions exhibited over an order of magnitude higher conductance than neutral states.
- Molecules exhibiting destructive quantum interference showed more pronounced conductance increases upon protonation.
- Experimental findings were corroborated by theoretical calculations predicting maximum conductance change when destructive interference is reduced.
Conclusions:
- Protonation is an effective strategy to modulate conductance in molecular junctions.
- Quantum interference plays a critical role in determining the conductance changes upon protonation.
- The developed theory accurately predicts the relationship between molecular structure, interference, and conductance modulation.
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