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Conformation-driven quantum interference effects mediated by through-space conjugation in self-assembled monolayers.

Marco Carlotti1, Andrii Kovalchuk1, Tobias Wächter2

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Area of Science:

  • Molecular electronics
  • Quantum interference
  • Solid-state physics

Background:

  • Tunnelling currents in molecular junctions are lower for cross-conjugated molecules compared to linear analogues.
  • This phenomenon is attributed to destructive quantum interference, an intrinsic molecular electronic property.

Purpose of the Study:

  • To investigate conformation-driven interference effects in molecular tunnelling junctions.
  • To explore through-space conjugation for controlling charge transport.

Main Methods:

  • Fabrication of large-area tunnelling junctions using self-assembled monolayers.
  • Trapping molecules in non-equilibrium conformations mimicking X-ray crystal structures.
  • Experimental observation of tunnelling currents and comparison with zero-bias simulations.

Main Results:

  • Experimental evidence for conformation-driven interference effects in through-space conjugated systems.
  • Absence of interference effects in equilibrium gas-phase conformations.
  • Demonstration of significantly lower tunnelling currents due to destructive interference.

Conclusions:

  • Through-space conjugation offers a mechanism to control quantum interference in molecular electronics.
  • Non-equilibrium molecular conformations are crucial for observing these interference effects.
  • This approach provides a pathway for tuning charge transport in solid-state molecular devices.