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A crown‐ether dithiol quaterthiophene  is synthesized and immobilized on gold surface by double covalent fixation. UV‐vis spectroscopy and cyclic voltammetry show that the corresponding dithioester precursor can complex Pb 2+  in solution and that this property is maintained for monolayers of the dithiol on gold. Current‐voltage measurements by eutectic GaIn drop contact on the monolayer show a significant increase (up to 1.6 × 10 3  times) of the current at low bias after Pb 2+  complexation.

A Crown‐Ether Loop‐Derivatized Oligothiophene Doubly Attached on Gold Surface as Cation‐Binding Switchable Molecular Junction