Understanding the charge transport properties of redox active metal-organic conjugated wires

Chemical Science
Donglei BuChun Y Liu

Abstract

Layer-by-layer assembly of the dirhodium complex [Rh2(O2CCH3)4] (Rh2) with linear N,N'-bidentate ligands pyrazine (LS) or 1,2-bis(4-pyridyl)ethene (LL) on a gold substrate has developed two series of redox active molecular wires, (Rh2LS) n @Au and (Rh2LL) n @Au (n = 1-6). By controlling the number of assembling cycles, the molecular wires in the two series vary systematically in length, as characterized by UV-vis spectroscopy, cyclic voltammetry and atomic force microscopy. The current-voltage characteristics recorded by conductive probe atomic force microscopy indicate a mechanistic transition for charge transport from voltage-driven to electrical field-driven in wires with n = 4, irrespective of the nature and length of the wires. Whilst weak length dependence of electrical resistance is observed for both series, (Rh2LL) n @Au wires exhibit smaller distance attenuation factors (β) in both the tunneling (β = 0.044 Å-1) and hopping (β = 0.003 Å-1) regimes, although in (Rh2LS) n @Au the electronic coupling between the adjacent Rh2 centers is stronger. DFT calculations reveal that these wires have a π-conjugated molecular backbone established through π(Rh2)-π(L) orbital interactions, and (Rh2LL) n @Au has a smaller ener...Continue Reading

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Citations

Jun 15, 2019·Chemical Communications : Chem Comm·Bruno M Aramburu-TrošeljAlejandro Cadranel
Oct 7, 2020·Nanoscale·Roméo BonnetDominique Vuillaume
Jul 11, 2020·Chemistry : a European Journal·Stephan LudwigWolfram Willy Seidel
Oct 26, 2018·Journal of the American Chemical Society·Yanxi ZhangRyan C Chiechi

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Methods Mentioned

BETA
atomic force microscopy
AFM
X-ray

Software Mentioned

Gaussian
Ray
VMD
POV

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