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Multiple-time-scale motion in molecularly linked nanoparticle arrays.

Christopher George1, Igal Szleifer, Mark Ratner

  • 1Department of Chemistry, Chemistry of Life Processes Institute, Northwestern University, Evanston, Illinois 60208, USA.

ACS Nano
|December 4, 2012
PubMed
Summary

Electron transport in quantum dot arrays is complex due to molecular motion. A combined theoretical approach reveals dynamic bond percolation governs electron transfer across these systems.

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Area of Science:

  • Molecular Electronics
  • Quantum Dot Arrays
  • Electron Transfer Dynamics

Background:

  • Electron transport through molecular junctions is crucial for molecular electronics.
  • Dynamical motion of molecules and quantum dots at finite temperatures complicates standard transport models.
  • Understanding these dynamics is key to designing efficient molecular electronic devices.

Purpose of the Study:

  • To investigate electron transport in a two-dimensional array of metallic quantum dots linked by mobile molecular bridges.
  • To develop a theoretical framework that accounts for the multiple time scales of dynamical processes influencing electronic transport.
  • To explore the applicability of dynamic bond percolation models to such systems.

Main Methods:

  • Employed a hybrid theoretical approach combining kinetic Monte Carlo, classical molecular dynamics, and quantum transport simulations.

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  • Modeled electron transfer in a system with mobile quantum dots and molecular linkers.
  • Analyzed the influence of molecular and quantum dot motion on charge transport.

    • Main Results:

    • Standard electron transfer approaches are insufficient due to coupled dynamics.
    • Electron transport exhibits characteristics of a dynamic bond percolation process.
    • Different dynamical effects become rate-limiting depending on the specific conditions and time scales.

    Conclusions:

    • A multi-timescale theoretical framework is necessary for accurate modeling of electron transport in dynamically disordered molecular arrays.
    • The dynamic bond percolation model provides a powerful scheme for understanding electron transfer in such complex systems.
    • This approach is applicable to various scenarios involving molecular arrays and single molecules with inherent disorder.