Precise Control of Single-phenanthrene Junction’s Conductance

The electronic transmission of fifteen potential configurations of single-phenanthrene junction has been theoretically investigated. The structures include para-para, para-meta, and meta-meta combined with phenyl pendant group and substituted nitrogen atom. The results show that the para-meta, which offers a tunable antiresonance in the HOMO-LUMO gap, is the most suitable for synthesizing nano-device. The antiresonance is susceptible (unsusceptible) to the heteromotif location at site four (five). Hence, our paper presents the appropriate hetero-motif conditions—type and location— to synthesize molecular devices with the desired electronic conductance. The study also deepen the understanding of the molecular conductance by demonstrating the active and inactive sites to create and tune antiresonances. It finally introduces the essential impact of connectivity, quantum interference, and aromaticity in controlling the conductance of single-phenanthrene junction.

Mechanical single-molecule potentiometers with large switching factors from ortho-pentaphenylene foldamers

Molecular potentiometers that can indicate displacement-conductance relationship, and predict and control molecular conductance are of significant importance but rarely developed. Herein, single-molecule potentiometers are designed based on ortho-pentaphenylene. The ortho-pentaphenylene derivatives with anchoring groups adopt multiple folded conformers and undergo conformational interconversion in solutions. Solvent-sensitive multiple conductance originating from different conformers is recorded by scanning tunneling microscopy break junction technique. These pseudo-elastic folded molecules can be stretched and compressed by mechanical force along with a variable conductance by up to two orders of magnitude, providing an impressively higher switching factor (114) than the reported values (ca. 1~25). The multichannel conductance governed by through-space and through-bond conducting pathways is rationalized as the charge transport mechanism for the folded ortho-pentaphenylene derivatives. These findings shed light on exploring robust single-molecule potentiometers based on helical structures, and are conducive to fundamental understanding of charge transport in higher-order helical molecules.

Substitution Pattern Controlled Charge Transport in BN-Embedded Aromatics-Based Single-Molecule Junctions

The understanding of charge transport at single-molecule level is a pre-requisite for the fabrication of molecular devices. Here, we systematically investigate the relation among molecular conductance, substitution pattern and stimuli...

The Anomalous Effect of Quantum Interference in Organic Spin Filters

The molecular topology in the single-molecular nano-junctions through which the de Broglie wave propagates plays a crucial role in controlling the molecular conductance. The enhancement and reduction of the conductance due to constructive and destructive Quantum Interference (QI) in para and meta connected molecules respectively has already been well established. Herein, we investigated the influence of QI on spin transport in the molecular junctions containing organic radicals as magnetic centres. The role of the localized spins on the QI as well as on spin filtering capability is investigated employing density functional theory in combination with non-equilibrium Green's function (NEGF-DFT) techniques. Various organic radicals including nitroxide (NO), phenoxy (PO) and methyl (CH2) radicals attached to the central benzene ring of pentacene with different terminal connections (para and meta) to gold electrodes are examined. Due to more obvious QI effects, para connected pentacene is found to be more conductive than meta one. Surprisingly, on incorporating a radical centre, along with spin filtering, a significant quenching of QI effects is observed which manifests itself in such a way that the conductance of meta coupled radicals is found to be more than para by two orders of magnitude. The decoherence induced by radical centre is analysed and discussed in terms of spin-spin coupling of radical's unpaired electron with the tunneling electrons.<br>

The Anomalous Effect of Quantum Interference in Organic Spin Filters

The molecular topology in the single-molecular nano-junctions through which the de Broglie wave propagates plays a crucial role in controlling the molecular conductance. The enhancement and reduction of the conductance due to constructive and destructive Quantum Interference (QI) in para and meta connected molecules respectively has already been well established. Herein, we investigated the influence of QI on spin transport in the molecular junctions containing organic radicals as magnetic centres. The role of the localized spins on the QI as well as on spin filtering capability is investigated employing density functional theory in combination with non-equilibrium Green's function (NEGF-DFT) techniques. Various organic radicals including nitroxide (NO), phenoxy (PO) and methyl (CH2) radicals attached to the central benzene ring of pentacene with different terminal connections (para and meta) to gold electrodes are examined. Due to more obvious QI effects, para connected pentacene is found to be more conductive than meta one. Surprisingly, on incorporating a radical centre, along with spin filtering, a significant quenching of QI effects is observed which manifests itself in such a way that the conductance of meta coupled radicals is found to be more than para by two orders of magnitude. The decoherence induced by radical centre is analysed and discussed in terms of spin-spin coupling of radical's unpaired electron with the tunneling electrons.<br>