Orbital Views of the Electron Transport in Molecular Devices

Yoshizawa, Kazunari; Tada, Tomofumi; Staykov, Aleksandar

doi:10.1021/ja800638t

Cited by 240 publications

(384 citation statements)

References 72 publications

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“…4,14,15 While conductance and interference patterns in alternant hydrocarbons have been the main focus, [14][15][16][17][18][19] little is known about how substitution patterns affect the single-molecule conductance properties of nonalternant hydrocarbons, 20 where quantum interference (QI) effects may not be predicted based on simple bond-counting models. 21,22 The optical properties and chemistry of alternant and non-alternant hydrocarbons vary widely with respect to each other. 20 A classical example is the comparison of naphthalene to azulene.…”

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confidence: 99%

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Breakdown of Interference Rules in Azulene, a Nonalternant Hydrocarbon

Xia

Capozzi²,

Wei³

et al. 2014

Nano Lett.

125

159

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We have designed and synthesized five azulene derivatives containing goldbinding groups at different points of connectivity within the azulene core to probe the effects of quantum interference through single-molecule conductance measurements. We compare conducting paths through the 5-membered ring, 7-membered ring, and across the long axis of azulene. We find that changing the points of connectivity in the azulene impacts the optical properties (as determined from UV-Vis absorption spectra) and the conductivity. Importantly, we show here that simple models cannot be used to predict quantum interference characteristics of non-alternant hydrocarbons. As an exemplary case, we show that azulene derivatives that are predicted to exhibit destructive interference based on widely accepted atom-counting models show a significant conductance at low biases. Although simple models to predict the low-bias conductance do not hold with all azulene derivatives, we show that the measured conductance trend for all molecules studied actually agrees with predictions based on the more complete GW calculations for model systems.

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confidence: 99%

“…25 Consequently, the single-molecule conductance patterns through naphthalene can also be reasoned with the MO picture and tight-binding energy transmission curves. 14,22 However, little is known about the effects of the substitution patterns of azulene on the single molecule conductance by "wiring" azulene through various points of connectivity ( Figure 1B). …”

mentioning

confidence: 99%

Breakdown of Interference Rules in Azulene, a Nonalternant Hydrocarbon

Xia

Capozzi²,

Wei³

et al. 2014

Nano Lett.

125

159

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“…7,[40][41][42][43] Here, we rationalise the QI interference features in terms of molecular orbitals and corresponding molecular energies. This has the advantage that in the weak molecule lead coupling limit this analysis can be generalised for the correlated electron case by considering so-called Dyson orbitals and energies.…”

Section: Resultsmentioning

confidence: 92%

Interference enhanced thermoelectricity in quinoid type structures

Strange

Seldenthuis

Verzijl

et al. 2015

The Journal of Chemical Physics

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Quantum interference (QI) effects in molecular junctions may be used to obtain large thermoelectric responses. We study the electrical conductance G and the thermoelectric response of a series of molecules featuring a quinoid core using density functional theory, as well as a semi-empirical interacting model Hamiltonian describing the π-system of the molecule which we treat in the GW approximation. Molecules with a quinoid type structure are shown to have two distinct destructive QI features close to the frontier orbital energies. These manifest themselves as two dips in the transmission, that remain separated, even when either electron donating or withdrawing side groups are added. We find that the position of the dips in the transmission and the frontier molecular levels can be chemically controlled by varying the electron donating or withdrawing character of the side groups as well as the conjugation length inside the molecule. This feature results in a very high thermoelectric power factor S 2 G and figure of merit ZT, where S is the Seebeck coefficient, making quinoid type molecules potential candidates for efficient thermoelectric devices. C 2015 AIP Publishing LLC. [http://dx

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“…Firstly, if the molecule and the electrodes have strong chemically bonds, then the electron densities of the molecule-electrode interfaces become high and electrons are less likely to pass through the interfaces; this will result in a small current being produced. 28,29,62 Secondly, single-molecule measurements invariably use chemically active nanostructures as electrodes; for example, considering that gold nanoparticles are often used as catalysts, 63,64 some chemical activity can be assumed even when using gold electrodes. If copper or silver electrodes were used instead, they would readily oxidize under ambient atmospheric conditions.…”

Section: Single-molecule Analysis Methodsmentioning

confidence: 99%

Single-Molecule Analysis Methods Using Nanogap Electrodes and Their Application to DNA Sequencing Technologies

Taniguchi

2017

Bulletin of the Chemical Society of Japan

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Single-molecule analysis methods facilitate the investigation of the properties of single-molecule junctions (SMJs), in which single molecules are connected between a pair of nanoelectrodes that use nanogap electrodes having a spacing of less than several nanometers. Various methods have been developed to investigate numerous useful parameters for SMJs; for example, the number of molecules connected between a pair of nanoelectrodes can be determined, the types and structures of single molecules can be revealed, localized temperatures within SMJs can be evaluated, and the Seebeck coefficient and the bond strength between single molecules and electrodes can be ascertained. Single-molecule analysis methods have also been used to analyze biopolymers in solutions, and this has resulted in single-molecule sequencing technologies being developed that can determine sequences of base molecules in DNA and RNA along with sequences of amino acids in peptides. Singlemolecule analysis methods are expected to develop into digital analysis techniques that can be used to investigate the physical and chemical properties of molecules at single-molecule resolutions.

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Orbital Views of the Electron Transport in Molecular Devices

Cited by 240 publications

References 72 publications

Breakdown of Interference Rules in Azulene, a Nonalternant Hydrocarbon

Breakdown of Interference Rules in Azulene, a Nonalternant Hydrocarbon

Interference enhanced thermoelectricity in quinoid type structures

Single-Molecule Analysis Methods Using Nanogap Electrodes and Their Application to DNA Sequencing Technologies

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