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We have to mention that it is not completely clear that sulfur is the best atom to couple to alkali leads. A complete study of the possible coupling atoms is beyond the scope of this work, but we do not expect the main conclusions to be affected by this point because in general the qualitative trends in the zero-bias transport characteristics do not depend too much on the coupling atom (Ref.).
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We have to mention that it is not completely clear that sulfur is the best atom to couple to alkali leads. A complete study of the possible coupling atoms is beyond the scope of this work, but we do not expect the main conclusions to be affected by this point because in general the qualitative trends in the zero-bias transport characteristics do not depend too much on the coupling atom (Ref.).
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Based on calculations with the BDT molecule, a SZP basis is enough to accurately describe the results of this work. We note that the inclusion of polarization orbitals is a key factor to correctly reproduce the states above the Fermi level, in particular the LUMO, whereas the inclusion of double zetas only produces a shift in the energy of the isolated systems which is corrected when they become coupled.
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58049106649
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We are aware that the position of this orbital is not exactly given by DFT (Refs.), but it is the trend in the change in the Fermi level and its movement from the middle of the gap toward higher-conductance values that is of particular interest.
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We are aware that the position of this orbital is not exactly given by DFT (Refs.), but it is the trend in the change in the Fermi level and its movement from the middle of the gap toward higher-conductance values that is of particular interest.
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58049106121
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note
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For K, Rb, and Cs the HOMO was so thin that the energy grid used to plot the transmission coefficients was not enough to represent it.
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58049098137
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note
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We would like to point out, however, that from an experimental point of view the use of alkali electrodes would be a difficult task due to the high reactivity of such materials.
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