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