We investigate vibron-assisted electron transport in single-molecule transistors containing an individual Fe4 Single-Molecule Magnet. We observe a strong suppression of the tunneling current at low bias in combination with vibron-assisted excitations. The observed features are explained by a strong electron-vibron coupling in the framework of the Franck-Condon model supported by density-functional theory.
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http://dx.doi.org/10.1021/nl500524w | DOI Listing |
Nat Electron
August 2023
Department of Information Technology and Electrical Engineering, ETH Zurich, Zurich, Switzerland.
Nat Mater
February 2023
Department of Materials, University of Oxford, Oxford, UK.
Only single-electron transistors with a certain level of cleanliness, where all states can be properly accessed, can be used for quantum experiments. To reveal their exceptional properties, carbon nanomaterials need to be stripped down to a single element: graphene has been exfoliated into a single sheet, and carbon nanotubes can reveal their vibrational, spin and quantum coherence properties only after being suspended across trenches. Molecular graphene nanoribbons now provide carbon nanostructures with single-atom precision but suffer from poor solubility, similar to carbon nanotubes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2019
Tianjin Key Laboratory of Molecular Optoelectronic Science, Department of Physics and Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, P. R. China.
We report an effective modulation of the quantum transport in molecular junctions consisting of aggregation-induced-emission(AIE)-active molecules. Theoretical simulations based on combined density functional theory and rate-equation method calculations show that the low-bias conductance of the junction with a single tetraphenylethylene (TPE) molecule can be completely suppressed by strong electron-vibration couplings, that is, the Franck-Condon blockade effect. It is mainly associated with the low-energy vibration modes, which is also the origin of the fluorescence quenching of the AIE molecule in solution.
View Article and Find Full Text PDFJ Chem Phys
September 2018
Department of Physics, McGill University, 3600 Rue University, Montréal, Québec H3A 2T8, Canada.
In this work, we explore Franck-Condon blockade in the "redox limit," where nuclear relaxation processes occur much faster than the rate of electron transfer. To this end, the quantized rate expressions for electron transfer are recast in terms of a quantized redox density of states (DOS) within a single phonon mode model. In the high temperature regime, this single-particle picture formulation of electron transfer is shown to agree well with the semi-classical rate and DOS expressions developed by Gerischer and Hopfield.
View Article and Find Full Text PDFJ Chem Phys
September 2017
College of Science and Engineering, James Cook University, Townsville, QLD 4811, Australia.
Quantum transport of electrons through a molecule is a series of individual electron tunneling events separated by stochastic waiting time intervals. We study the emergence of temporal correlations between successive waiting times for the electron transport in a vibrating molecular junction. Using the master equation approach, we compute the joint probability distribution for waiting times of two successive tunneling events.
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