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Interfacial Hopping Integral as a Predictive Descriptor for Electron Transport: Saturated Alkane Junctions.

Hao Howard Peng1, Chih-Hsun Lin1, Po-Wei Tung1

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We introduce the interfacial hopping integral (t_eld-mol) to quantify orbital overlap, predicting single-molecule conductance. This new descriptor explains variations in conductance for alkane molecules based on their orientation.

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Area of Science:

  • Surface Science and Nanotechnology
  • Molecular Electronics
  • Quantum Transport

Background:

  • Electron transport across interfaces is crucial for many physical phenomena.
  • Orbital overlap is a known factor influencing electron transport, but its experimental measurement is challenging.
  • Understanding single-molecule conductance requires precise quantification of interfacial electronic coupling.

Purpose of the Study:

  • To experimentally establish and validate the interfacial hopping integral (t_eld-mol) as a predictive descriptor for single-molecule conductance.
  • To correlate molecular conductance with quantifiable parameters like molecular tilt (tilt_mol) in functionalized alkane junctions.
  • To develop a theoretical model that explains and generalizes conductance variations in diverse molecular junctions.

Main Methods:

  • Utilized scanning tunneling microscopy and molecular-junction mapping techniques.
  • Correlated single-molecule conductance measurements with molecular tilt (tilt_mol) for π- and σ-type headgroups.
  • Employed a tight-binding model with Newns-Anderson-Grimley theory to analyze electron transport across metal-molecule interfaces.

Main Results:

  • Successfully extracted the interfacial hopping integral (t_eld-mol), quantifying orbital overlap between contacting atoms.
  • Generated conductance heatmaps using a theoretical model that qualitatively match experimental observations.
  • Rationalized existing literature findings on alkanedithiol conductance, linking them to molecular tilt and interfacial hopping integral variations.

Conclusions:

  • The interfacial hopping integral (t_eld-mol) serves as a robust, experimentally validated descriptor for single-molecule conductance.
  • Molecular tilt (tilt_mol) significantly influences conductance by modulating the interfacial hopping integral.
  • The developed theoretical framework provides a generalized approach to understanding electron transport in various molecular junctions.