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Conformational fluctuations and quantum interference significantly impact single-molecule junction electrical conductance. Including these effects improves theoretical predictions, revealing quantum interference signatures persist despite molecular motion.

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Area of Science:

  • Molecular electronics
  • Quantum chemistry
  • Condensed matter physics

Background:

  • Single-molecule break junctions are crucial for molecular electronics.
  • Understanding electrical conductance requires accounting for molecular structure and dynamics.
  • Quantum interference effects can dramatically alter molecular conductance.

Purpose of the Study:

  • To investigate the interplay of conformational fluctuations and quantum interference on molecular conductance.
  • To compare theoretical predictions with experimental data for methylsulfide-functionalized diphenyloligoenes.
  • To assess the impact of conformational averaging on theoretical models.

Main Methods:

  • Density functional theory (DFT) calculations for electronic structure.
  • Classical molecular dynamics simulations to generate conformational ensembles.
  • Computation of conformationally-averaged conductance.

Main Results:

  • Distinct transport regimes observed during junction evolution.
  • Quantum interference signatures are robust against conformational fluctuations.
  • Conformational averaging significantly enhances agreement between theory and experiment.

Conclusions:

  • Conformational dynamics are essential for accurate modeling of molecular conductance.
  • Quantum interference remains a key factor even with molecular flexibility.
  • Combined theoretical approaches provide reliable predictions for molecular junctions.