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Scale-Up of Room-Temperature Constructive Quantum Interference from Single Molecules to Self-Assembled Molecular-Electronic Films

Xintai Wang, Troy L. R. Bennett, Ali Ismael, Luke A. Wilkinson, Joseph Hamill, Andrew J. P. White, Iain Grace, Oleg Kolosov, Tim Albrecht, Benjamin J. Robinson, Nicholas J. Long, L. F. Cohen, Colin J. Lambert

2020Journal of the American Chemical Society55 citationsDOIOpen Access PDF

Abstract

QI (CQI) in cross-plane transport through SAMs and assess its influence on cross-plane thermoelectricity in SAMs. It is known that the electrical conductance of single molecules can be controlled in a deterministic manner, by chemically varying their connectivity to external electrodes. Here, by employing synthetic methodologies to vary the connectivity of terminal anchor groups around aromatic anthracene cores, and by forming SAMs of the resulting molecules, we clearly demonstrate that this signature of CQI can be translated into SAM-on-gold molecular films. We show that the conductance of vertical molecular junctions formed from anthracene-based molecules with two different connectivities differ by a factor of approximately 16, in agreement with theoretical predictions for their conductance ratio based on CQI effects within the core. We also demonstrate that for molecules with thioether anchor groups, the Seebeck coefficient of such films is connectivity dependent and with an appropriate choice of connectivity can be boosted by ∼50%. This demonstration of QI and its influence on thermoelectricity in SAMs represents a critical step toward functional ultra-thin-film devices for future thermoelectric and molecular-scale electronics applications.

Topics & Concepts

ChemistryConductanceMoleculeThermoelectric effectAnthraceneChemical physicsMonolayerNanotechnologyElectrical resistance and conductanceCondensed matter physicsMaterials scienceQuantum mechanicsOrganic chemistryPhysicsBiochemistryMolecular Junctions and NanostructuresAdvanced Thermoelectric Materials and DevicesQuantum and electron transport phenomena