Issue 30, 2021

Destructive quantum interference in heterocyclic alkanes: the search for ultra-short molecular insulators

Abstract

Designing highly insulating sub-nanometer molecules is difficult because tunneling conductance increases exponentially with decreasing molecular length. This challenge is further enhanced by the fact that most molecules cannot achieve full conductance suppression with destructive quantum interference. Here, we present results for a series of small saturated heterocyclic alkanes where we show that conductance is suppressed due to destructive interference. Using the STM-BJ technique and density functional theory calculations, we confirm that their single-molecule junction conductance is lower than analogous alkanes of similar length. We rationalize the suppression of conductance in the junctions through analysis of the computed ballistic current density. We find there are highly symmetric ring currents, which reverse direction at the antiresonance in the Landauer transmission near the Fermi energy. This pattern has not been seen in earlier studies of larger bicyclic systems exhibiting interference effects and constitutes clear-cut evidence of destructive σ-interference. The finding of heterocyclic alkanes with destructive quantum interference charts a pathway for chemical design of short molecular insulators using organic molecules.

Graphical abstract: Destructive quantum interference in heterocyclic alkanes: the search for ultra-short molecular insulators

Supplementary files

Article information

Article type
Edge Article
Submitted
23 4 2021
Accepted
25 6 2021
First published
30 6 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2021,12, 10299-10305

Destructive quantum interference in heterocyclic alkanes: the search for ultra-short molecular insulators

B. Zhang, M. H. Garner, L. Li, L. M. Campos, G. C. Solomon and L. Venkataraman, Chem. Sci., 2021, 12, 10299 DOI: 10.1039/D1SC02287C

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