Simplifying the conductance profiles of molecular junctions: the use of the trimethylsilylethynyl moiety as a molecule–gold contact

Marqués‐González, Santiago; Yufit, Dmitry S.; Howard, Judith A. K.; Martı́n, Santiago; Osorio, Henrry M.; García‐Suárez, Víctor M.; Nichols, Richard J.; Higgins, Simon J.; Cea, Pilar; Low, Paul J.

doi:10.1039/c2dt31825c

Cited by 84 publications

(87 citation statements)

References 27 publications

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“…Similarly, junctions can be formed with a terminal acetylene (alkyne, -C≡C-H) group (73,74). It has also been shown to be possible to form junctions with terminal trimethylsilylethynyl (TMSE, -C≡C-SiMe 3 ) and gold electrodes (75)(76)(77). Trimethylsilylethynyl had been previously shown to be a contacting group for forming stable SAMs on Au (110,(78)(79)(80)(81).…”

Section: Anchoring Groups and Contactsmentioning

confidence: 96%

Single-Molecule Electronics: Chemical and Analytical Perspectives

Nichols

Higgins

2015

Annual Rev. Anal. Chem.

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It is now possible to measure the electrical properties of single molecules using a variety of techniques including scanning probe microcopies and mechanically controlled break junctions. Such measurements can be made across a wide range of environments including ambient conditions, organic liquids, ionic liquids, aqueous solutions, electrolytes, and ultra high vacuum. This has given new insights into charge transport across molecule electrical junctions, and these experimental methods have been complemented with increasingly sophisticated theory. This article reviews progress in single-molecule electronics from a chemical perspective and discusses topics such as the molecule-surface coupling in electrical junctions, chemical control, and supramolecular interactions in junctions and gating charge transport. The article concludes with an outlook regarding chemical analysis based on single-molecule conductance.

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Section: Anchoring Groups and Contactsmentioning

confidence: 96%

Single-Molecule Electronics: Chemical and Analytical Perspectives

Nichols

Higgins

2015

Annual Rev. Anal. Chem.

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“…7 Au-pyridyl contacts, such as the Au-44BP bond, have been shown to provide reproducible junctions for which two conductance values can be distinguished due to different binding geometries. [8][9][10] However, despite significant progress investigating different chemical linker groups 9,[11][12][13][14][15][16][17][18] there have been few previous attempts to broaden the range of metal electrodes studied.…”

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confidence: 99%

Single-Molecule Electrochemical Transistor Utilizing a Nickel-Pyridyl Spinterface

et al. 2014

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Using a scanning tunnelling microscope break-junction technique, we produce 4,4'-bipyridine (44BP) single-molecule junctions with Ni and Au contacts. Electrochemical control is used to prevent Ni oxidation, and to modulate the conductance of the devices via non-redox gating -the first time this has been shown using non-Au contacts. Remarkably the conductance and gain of the resulting Ni-44BP-Ni electrochemical transistors is significantly higher than analogous Au-based devices. Ab-initio calculations reveal that this behaviour arises because charge transport is mediated by spin-polarized Ni d -electrons, which hybridize strongly with molecular orbitals to form a 'spinterface'.Our results highlight the important role of the contact material for single-molecule devices, and show that it can be varied to provide control of charge and spin transport. KeywordsSingle-molecule, Break-junction, Electrochemical gating, Spintronics, Density functional theory, Metal-molecule interface Main TextSingle-molecule transistor behaviour can be achieved using a gate electrode to control the energy levels of a molecule bridging two metallic electrodes. 1 This gate can be provided electrochemically using the double layer potential existing at the metal-electrolyte interface (Fig. 1a). An electrochemical gate avoids the complex fabrication of solid-state threeterminal molecular devices, can operate in room temperature liquid environments, and can produce high gate efficiencies thanks to the large electric fields which are achievable. There has been significant interest in redox active molecules such as viologens as candidates for electrochemical transistors, 2-4 however the gating of non-redox molecules has only recently been demonstrated using Au electrodes by Li et al. 5 with 4,4'-bipyridine (44BP) molecules,

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“…Recent works on the trimethylsilylethynyl group (R-C≡C-Si-(CH 3 ) 3 ) have demonstrated chemisorption of this functional group on gold surfaces [79][80][81] with SAMs exhibiting a high surface coverage [82] and similar electrical characteristics to amine (R-NH 2 ) contacts. In addition, single molecules exhibit an unique conductance profile for this contacting group [82]. However, further work is needed to clarify the nature of this terminal group-metal interaction.…”

Section: Self-assembled Monolayers On Metal Surfacesmentioning

confidence: 98%

Nanofabrication techniques of highly organized monolayers sandwiched between two electrodes for molecular electronics

2014

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Molecular electronics [1,2] is a promising field of research based on the idea that a single molecule or two dimensional assemblies of molecules (monomolecular films) can work as wires, switches, rectifiers, etc. Molecules are the smallest functional units and therefore it is expected that the use of molecules will permit to catch up with the limits of miniaturization (MM: more Moore), with an increase in device density by a factor of several orders of magnitude compared to today's state of the art. At the same time due to quantum effects novel and remarkable properties of organic and organometallic compounds at the nanoscale devices will result in increased performance (MtM: more than Moore) together with the appearance of new functions not possible with conventional semiconductors, and also cheaper devices due to the non-dependence of expensive materials used today in CMOS (complementary metal-oxide semiconductor) technology such as hafnium oxide. Nowadays, the number of research groups from different disciplines of science contributing to molecular electronics is gradually growing, and this field is becoming of great scientific and technological interest [1,3-8]. Since the seminal work of Aviram and Ratner in 1974 who firstly suggested that a single molecule could function as a rectifier [9], molecules have been experimentally demonstrated to work as switches, molecular wires or rectifiers, and a new field of opportunities is opened due to the understanding of electron transport through single entities or assemblies of molecules and expansion towards work on molecular spintronics, vibronic effects, excitation of the molecular junction with polarized light, quantum interference and decoherence, molecular chirality, molecular stretching and distortion as well as work on thermoelectric response in molecular junctions.Abstract: It is expected that molecular electronics, i.e., the use of molecules as critical functional elements in electronic devices, will lead in the near future to an industrial exploitable novel technology, which will open new routes to high value-added electronic products. However, despite the enormous advances in this field several scientific and technological challenges should be surmounted before molecular electronics can be implemented in the market. Among these challenges are the fabrication of reliable, robust and uniform contacts between molecules and electrodes, the deposition of the second (top) contact electrode, and development of assembly strategies for precise placement of molecular materials within device structures. This review covers advances in nanofabrication techniques used for the assembly of monomolecular films onto conducting or semiconducting substrates as well as recent methods developed for the deposition of the top contact electrode highlighting the advantages and limitations of the several approaches used in the literature. This contribution also aims to define areas of outstanding challenges in the nanofabrication of monomolecular layers sandwiched between two electro...

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Simplifying the conductance profiles of molecular junctions: the use of the trimethylsilylethynyl moiety as a molecule–gold contact

Cited by 84 publications

References 27 publications

Single-Molecule Electronics: Chemical and Analytical Perspectives

Single-Molecule Electronics: Chemical and Analytical Perspectives

Single-Molecule Electrochemical Transistor Utilizing a Nickel-Pyridyl Spinterface

Nanofabrication techniques of highly organized monolayers sandwiched between two electrodes for molecular electronics

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