Understanding and Controlling Crosstalk between Parallel Molecular Wires

Reuter, Matthew G.; Solomon, Gemma C.; Hansen, Thorsten; Seideman, Tamar; Ratner, Mark A.

doi:10.1021/jz200658h

Cited by 33 publications

(70 citation statements)

References 43 publications

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“…While the calculations support that the linear and cross-conjugated forms, promoted by various local environments, could be the origin of the broad conductance histograms of the D–A molecules, we will now discuss some other possible explanations. Thus, crosstalk and cooperative effects 29 30 31 32 for transport mechanisms between molecular wires connected to the same gold electrodes is relevant to consider. A theoretical study by Dubi 32 is able to explain a lower conductance of molecules in self-assembled monolayers 33 by in-plane dephasing, while Akkerman and de Boer 34 first of all ascribe differences between single-molecule and self-assembled monolayer experiments to a difference in contacts.…”

Section: Discussionmentioning

confidence: 99%

Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments

et al. 2015

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The ability of molecules to change colour on account of changes in solvent polarity is known as solvatochromism and used spectroscopically to characterize charge-transfer transitions in donor–acceptor molecules. Here we report that donor–acceptor-substituted molecular wires also exhibit distinct properties in single-molecule electronics under the influence of a bias voltage, but in absence of solvent. Two oligo(phenyleneethynylene) wires with donor–acceptor substitution on the central ring (cruciform-like) exhibit remarkably broad conductance peaks measured by the mechanically controlled break-junction technique with gold contacts, in contrast to the sharp peak of simpler molecules. From a theoretical analysis, we explain this by different degrees of charge delocalization and hence cross-conjugation at the central ring. Thus, small variations in the local environment promote the quinoid resonance form (off), the linearly conjugated (on) or any form in between. This shows how the conductance of donor–acceptor cruciforms is tuned by small changes in the environment.

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Section: Discussionmentioning

confidence: 99%

Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments

et al. 2015

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“…Suppose that two molecules are caught in the junction at the same time: Is the current going through the two molecules the same as twice the current through a single molecule? Previous theoretical studies have shown that the transport through two or more molecules connected in parallel (which interact via their joint linkage to the electrodes, or directly with each other) can result in transport that is larger than, equal to, or smaller than twice the transport through a single molecule. This effect can be understood in analogy with an optical double‐slit experiment, where quantum coherence can mix the transport paths, giving twice the conductance for complete constructive interference and close to zero for complete destructive interference.…”

Section: Where We Have Beenmentioning

confidence: 99%

Forty years of molecular electronics: Non‐equilibrium heat and charge transport at the nanoscale

Bergfield

Ratner

2013

Physica Status Solidi (b)

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The “Quo Vadis?” meeting in Bremen (March 2013) was a spectacular opportunity for people involved in molecular electronics to catch up on the latest, to think back, and to project into the future. This manuscript is divided into two halves. In the first half, we address some of the history and where the field has advanced in the areas of measuring, modeling, making, and understanding materials. We review some big ideas that have animated the field of molecular electronics since its beginning, and are at the height of interest and accomplishment at the moment. Then, we discuss six major areas where the field is evolving, and in which we expect to see very exciting work in the years and decades ahead. As a representative of one of the neer themes, the second half of the paper is devoted to molecular thermoelectrics. It contains some formalism, some results, some experimental comparison, and some intriguing conceptual questions, both for pure science and for device applications. An artist's rendition of a self‐assembled monolayer of polyphenylether molecules on Au contacted by a Au STM.

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“…First, we can connect the wires in parallel and explore the "cooperative effects" between conduction channels. [83,84,[86][87][88][89][90] Second, we can connect the wires in series and examine the effects of "molecular length" on conductance. [91][92][93][94][95][96][97] We discuss each of these approaches in turn and then comment on their relation to locally ordered molecular materials.…”

Section: Electronic Transportmentioning

confidence: 99%

“…These changes in the transmission (per channel) indicate crosstalk between the channels, which is an interference effect between the direct (e.g., pÀp coupling) and electrode-mediated interchannel interactions. [83] Ultimately, the transmission spectra converge as n approaches 1, giving rise to a pseudo-Ohms law, G n parallel = nG 1 eff , in which G n parallel is the conductance through n parallel wires and G 1 eff is an effective one-channel conductance. [84,88] This pseudo-Ohms law has been experimentally validated, [98] and, as suggested in Figure 4a, G 1 eff is not required to be the same as G 1 .…”

Section: Electronic Transportmentioning

confidence: 99%

Emergent Properties in Locally Ordered Molecular Materials

Jackson

Savoie

Reuter

et al. 2014

Israel Journal of Chemistry

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The two classic structural classifications of solid matter, crystalline and amorphous, are quite useful for inorganic solids, from antimony trichloride to zinc dibromide and beyond. However, for many molecular materials, especially those based on components containing ten or more non‐hydrogen atoms, ordered single crystals are less common, and intermediate structures that are neither amorphous nor crystalline frequently dominate. Herein, we discuss several situations in which there is local (or partial) ordering in such molecular materials. These materials go beyond the standard concepts concerning polymers and must account for imperfect but substantial local ordering, such as that caused by weak intermolecular interactions (e.g., π stacking, H‐bonding, and/or dispersion forces). This local ordering has important implications for, and applications in, materials properties: we specifically consider dielectric response, electron transport, and exciton transfer. Finally, we discuss the fundamental importance of the effective dimensionality of partially ordered domains in molecular materials.

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Understanding and Controlling Crosstalk between Parallel Molecular Wires

Cited by 33 publications

References 43 publications

Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments

Tracking molecular resonance forms of donor–acceptor push–pull molecules by single-molecule conductance experiments

Forty years of molecular electronics: Non‐equilibrium heat and charge transport at the nanoscale

Emergent Properties in Locally Ordered Molecular Materials

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