Using self-energy-corrected density functional theory (DFT) and a coherentscattering-state approach, we explain current-voltage (IV) measurements of fourpyridine-Au and amine-Au linked molecular junctions with quantitative accuracy.Parameter-free many-electron self-energy corrections to DFT Kohn-Shameigenvalues are demonstrated to lead to excellent agreement with experiments atfinite bias, improving upon order-of-magnitude errors in currents obtained withstandard DFT approaches. We further propose an approximate route for predictionof quantitative IV characteristics for both symmetric and asymmetric molecularjunctions based on linear response theory and knowledge of the Stark shifts ofjunction resonance energies. Our work demonstrates that a quantitative,computationally inexpensive description of coherent transport in molecularjunctions is readily achievable, enabling new understanding and control ofcharge transport properties of molecular-scale interfaces at large biasvoltages.
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