Stretching helical molecular springs: the peculiar evolution of electron transport in helicene junctions

Abstract

Single-molecule junctions represent electromechanical systems at the edge of device miniaturization. Despite extensive studies on the interplay between mechanical manipulation and electron transport in molecular junctions, a thorough understanding of conducting molecular springs remains elusive. Here, we investigate the impact of mechanical elongation and compression on the electron transport and electronic structure of helicene-based spring-like single-molecule junctions, utilizing 2,2'-dithiol-[6]helicene and thioacetyl-[13]helicene molecules bridging two gold electrodes. We observe robust, reversible U-shaped conductance variations with interelectrode distance. Ab-initio electronic structure and quantum transport calculations reveal that this behavior stems from destructive quantum interference, induced mainly by modifications of the coupling at the metal-molecule interface as a peculiar outcome of the helical backbone deformation. These findings highlight the central role of the helical geometry in combination with contact properties in the electromechanical response of conducting molecular springs, offering insights for designing functional electromechanical devices that leverage similar mechanisms.