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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Nanoscience

Background:

  • Electron transport in molecular junctions is crucial for molecular electronics.
  • Solvent effects significantly influence molecular junction properties but are complex to model.
  • Controlling current via solvent stimuli offers a pathway for tunable molecular devices.

Purpose of the Study:

  • To develop a theoretical model for electron transport in molecular junctions considering dynamical solvent effects.
  • To investigate how solvent-molecule interactions, including dipole reorientation and viscosity, modulate electrical current.
  • To explore the potential of solvents as external stimuli for controlling charge transport.

Main Methods:

  • Developed a model incorporating dynamical solvent-molecule interactions within non-equilibrium Green's function (NEGF) calculations.
  • Treated the solvent as a stochastically reorienting macroscopic dipole interacting with tunneling electrons.
  • Solved Keldysh-Kadanoff-Baym equations in the time domain, employing the Furutsu-Novikov method for stochastic averaging.
  • Utilized wideband approximation and classical treatment of solvent degrees of freedom.

Main Results:

  • The model successfully captures the influence of solvent dynamics on electron transport.
  • Demonstrated that solvent viscosity, in addition to electrostatic interactions, can control junction electrical properties.
  • Showed that alignment of the solvent's dipole moment breaks particle-hole symmetry, selectively favoring electron or hole transport.

Conclusions:

  • Dynamical solvent effects are critical for understanding and controlling electron transport in molecular junctions.
  • Solvent properties like viscosity and dipole reorientation provide tunable parameters for molecular electronic devices.
  • The developed theoretical framework enables accurate prediction of solvent-modulated charge transport.