Extending the Newns-Anderson model to allow nanotransport studies through molecules with floppy degrees of freedom

Abstract

The Newns-Anderson model is ubiquitous in studies of the molecular transport in the presence of solvent (outer) reorganization. The present work demonstrates that intramolecular reorganization can also be significant for the transport through molecules with floppy degrees of freedom, for which the Newns-Anderson model can be extended. The expressions of the model parameters deduced from electronic structure calculations for (4, 4')-bipyridine (44BPY) quantitatively differ from those characteristic for outer reorganization due to strong intramolecular anharmonicities. These expressions can be utilized as input in transport calculations for 44BPY-based molecular junctions of experimental interest [Science 301 (2003) 203, J. Am. Chem. Soc. 130 (2008) 16045, Nano Lett. 12 (2012) 354].

arXiv commentaccepted for publication in EPL (Europhys. Lett.)

References in corpus (12)

• Kondo Physics in a Single Electron Transistor
• Dependence of Single Molecule Junction Conductance on Molecular Conformation
• Mechanically-Controlled Binary Conductance Switching of a Single-Molecule Junction
• Simultaneous Determination of Conductance and Thermopower of Single Molecule Junctions
• Polarization-induced renormalization of molecular levels at metallic and semiconducting surfaces
• Ambipolar transition voltage spectroscopy: analytical results and experimental agreement
• Vibrational nonequilibrium effects in the conductance of single-molecules with multiple electronic states
• Forces and conductances in a single-molecule bipyridine junction
• Mode-selective vibrational excitation induced by nonequilibrium transport processes in single-molecule junctions
• Sources of negative differential resistance in electric nanotransport
• Studying the single--electron transistor by photoionization
• Far-infrared absorption in single-electron transistors: Theoretical results and experiment proposal

Cited by in corpus (7)

• A quantum chemical study from a molecular perspective: ionization and electron attachment energies for species often used to fabricate single-molecule junctions
• Adsorption-Induced Solvent-Based Electrostatic Gating of Charge Transport through Molecular Junctions
• (4,4')-Bipyridine in Vacuo and in Solvents: A Quantum Chemical Study of a Prototypical Floppy Molecule From a Molecular Transport Perspective
• Alternation of Singlet and Triplet States in Carbon-Based Chain Molecules and Its Astrochemical Implications. Results of an Extensive Theoretical Study
• Quantifying the relative molecular orbital alignment for molecular junctions with similar chemical linkage to electrodes
• Electrochemical setup - a unique chance to simultaneously control orbital energies and vibrational properties of single-molecule junctions with unprecedented efficiency
• Why Ortho- and Para-Hydroxy Metabolites Can Scavenge Free Radicals that the Parent Atorvastatin Cannot? Important Pharmacologic Insight from Quantum Chemistry