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Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes.

ABSTRACT: The performance of nanoelectronic and molecular electronic devices relies strongly on the employed functional units and their addressability, which is often a matter of appropriate interfaces and device design. Here, we compare two promising designs to build solid-state electronic devices utilizing the same functional unit. Optically addressable Ru-terpyridine complexes were incorporated in supramolecular wires or employed as ligands of gold nanoparticles and contacted by nanoelectrodes. The resulting small-area nanodevices were thoroughly electrically characterized as a function of temperature and light exposure. Differences in the resulting device conductance could be attributed to the device design and the respective transport mechanism, that is, thermally activated hopping conduction in the case of Ru-terpyridine wire devices or sequential tunneling in nanoparticle-based devices. Furthermore, the conductance switching of nanoparticle-based devices upon 530 nm irradiation was attributed to plasmon-induced metal-to-ligand charge transfer in the Ru-terpyridine complexes used as switching ligands. Finally, our results reveal a superior device performance of nanoparticle-based devices compared to molecular wire devices based on Ru-terpyridine complexes as functional units.

SUBMITTER: Mennicken M

PROVIDER: S-EPMC8895035 | biostudies-literature | 2022

REPOSITORIES: biostudies-literature

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Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes.

Mennicken Max M Peter Sophia Katharina SK Kaulen Corinna C Simon Ulrich U Karthäuser Silvia S

Beilstein journal of nanotechnology 20220215

The performance of nanoelectronic and molecular electronic devices relies strongly on the employed functional units and their addressability, which is often a matter of appropriate interfaces and device design. Here, we compare two promising designs to build solid-state electronic devices utilizing the same functional unit. Optically addressable Ru-terpyridine complexes were incorporated in supramolecular wires or employed as ligands of gold nanoparticles and contacted by nanoelectrodes. The res ...[more]

PMID: 35281628

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Project description:The series of complexes [XRu(CO)(L-L)(L')2][PF6] (X = H, TFA, Cl; L-L = 2,2'-bipyridyl, 1,10-phenanthroline, 5-amino-1,10-phenanthroline and 4,4'-dicarboxylic-2,2'-bipyridyl; L'2 = 2PPh3, Ph2 PC2H4PPh2, Ph2PCH═CHPPh2) have been synthesized from the starting complex K[Ru(CO)3(TFA)3] (TFA = CF3CO2) by first reacting with the phosphine ligand, followed by reaction with the L-L and anion exchange with NaPF6. In the case of L-L = phenanthroline and L'2 = 2PPh3, the neutral complex Ru(Ph3P)(CO)(1,10-phenanthroline)( TFA)2 is also obtained and its solid state structure is reported. Solid state structures are also reported for the cationic complexes where L-L = phenanthroline, L2 = 2PPh3 and X = Cl and for L-L = 2,2'-bipyridyl, L2 = 2PPh3 and X = H. All the complexes were characterized in solution by a combination of 1H and 31P NMR, IR, mass spectrometry and elemental analyses. The purpose of the project was to synthesize a series of complexes that exhibit a range of excited-state lifetimes and that have large Stokes shifts, high quantum yields and high intrinsic polarizations associated with their metal-to-ligand charge-transfer (MLCT) emissions. To a large degree these goals have been realized in that excited-state lifetimes in the range of 100 ns to over 1 μs are observed. The lifetimes are sensitive to both solvent and the presence of oxygen. The measured quantum yields and intrinsic anisotropies are higher than for previously reported Ru(II) complexes. Interestingly, the neutral complex with one phosphine ligand shows no MLCT emission. Under the conditions of synthesis some of the initially formed complexes with X = TFA are converted to the corresponding hydrides or in the presence of chlorinated solvents to the corresponding chlorides, testifying to the lability of the TFA Ligand. The compounds show multiple reduction potentials which are chemically and electrochemically reversible in a few cases as examined by cyclic voltammetry. The relationships between the observed photophysical properties of the complexes and the nature of the ligands on the Ru(II) is discussed.

Dataset Information

Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes.

Publications

Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes.

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