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Electrochemical gate-controlled electron transport of redox-active single perylene bisimide molecular junctions

C Li1,2, A Mishchenko1, Z Li1, I Pobelov1,2, Th Wandlowski1,2, X Q Li3, F Würthner3, A Bagrets4,5 and F Evers4,5

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We report a scanning tunneling microscopy (STM) experiment in an electrochemical environment which studies a prototype molecular switch. The target molecules were perylene tetracarboxylic acid bisimides modified with pyridine (P-PBI) and methylthiol (T-PBI) linker groups and with bulky tert-butyl-phenoxy substituents in the bay area. At a fixed bias voltage, we can control the transport current through a symmetric molecular wire Au|P-PBI(T-PBI)|Au by variation of the electrochemical 'gate' potential. The current increases by up to two orders of magnitude. The conductances of the P-PBI junctions are typically a factor 3 larger than those of T-PBI. A theoretical analysis explains this effect as a consequence of shifting the lowest unoccupied perylene level (LUMO) in or out of the bias window when tuning the electrochemical gate potential VG. The difference in on/off ratios reflects the variation of hybridization of the LUMO with the electrode states with the anchor groups. IT–ES(T) curves of asymmetric molecular junctions formed between a bare Au STM tip and a T-PBI (P-PBI) modified Au(111) electrode in an aqueous electrolyte exhibit a pronounced maximum in the tunneling current at −0.740, which is close to the formal potential of the surface-confined molecules. The experimental data were explained by a sequential two-step electron transfer process.


PACS

73.40.Gk Tunneling

82.45.Gj Electrolytes

68.37.Ef Scanning tunneling microscopy (including chemistry induced with STM)

82.45.Fk Electrodes

Subjects

Surfaces, interfaces and thin films

Chemical physics and physical chemistry

Dates

Issue 37 (17 September 2008)

Received 15 February 2008

Published 26 August 2008



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