Interference and Molecular Transport-A Dynamical View: Time-Dependent Analysis of Disubstituted Benzenes

J Phys Chem Lett. 2014 Aug 7;5(15):2748-52. doi: 10.1021/jz5007143. Epub 2014 Jul 29.


The primary issue in molecular electronics is measuring and understanding how electrons travel through a single molecule strung between two electrodes. A key area involves electronic interference that occurs when electrons can follow more than one pathway through the molecular entity. When the phases developed along parallel pathways are inequivalent, interference effects can substantially reduce overall conductance. This fundamentally interesting issue can be understood using classical rules of physical organic chemistry, and the subject has been examined broadly. However, there has been little dynamical study of such interference effects. Here, we use the simplest electronic structure model to examine the coherent time-dependent transport through meta- and para-linked benzene circuits, and the effects of decoherence. We find that the phase-caused coherence/decoherence behavior is established very quickly (femtoseconds), that the localized dephasing at any site reduces the destructive interference of the meta-linked species (raising the conductance), and that thermal effects are essentially ineffectual for removing coherence effects.

Keywords: decoherence; molecular electronics; quantum interference; quantum transport; transient current; transistor.