Negative differential resistance at sequential single-electron tunnelling through atoms and molecules.

We have carried out calculations of electron transport in single-electron transistors using single atoms or small molecules as single-electron islands. The theory is based on a combination of (i) the general theory of the sequential single-electron transport through objects with a quantized energy spectrum, developed by Averin and Korotkov, (ii) the ab initio calculation of molecular orbitals and energy spectra within the density functional theory framework (using the NRLMOL software package), and (iii) Bardeen's approximation for the rate of tunnelling due to wavefunction overlap. The results show, in particular, that dc I-V curves of molecular-scale single-electron transistors typically have extended branches with negative differential resistance. This effect is due to the enhancement of one of the two tunnelling barriers of the transistor by the source-drain electric field, and apparently has already been observed experimentally by at least two groups. In conclusion, the possibility of using this effect for increasing the density and performance of hybrid semiconductor/nanodevice integrated circuits is discussed in brief.