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All density functional calculations of single-molecule transport to date haveused continuous exchange-correlation approximations. The lack of derivativediscontinuity in such calculations leads to the erroneous prediction ofmetallic transport for insulating molecules. A simple and computationallyundemanding atomic self-interaction correction greatly improves the agreementwith experiment for the prototype Au/dithiolated-benzene/Au junction.

Self-Interaction Errors in Density-Functional Calculations of Electronic Transport