Understanding the influence of vibrational motion of the atoms on electronic transitions in molecules constitutes a cornerstone of quantum physics, as epitomized by the Franck-Condon principle 1,2 of spectroscopy. Recent advances in building molecular-electronics devices 3 and nanoelectromechanical systems 4 open a new arena for studying the interaction between mechanical and electronic degrees of freedom in transport at the single-molecule level. The tunneling of electrons through molecules or suspended quantum dots 5,6 has been shown to excite vibrational modes, or vibrons 7-9,6 . Beyond this effect, theory predicts that strong electron-vibron coupling dramatically suppresses the current flow at low biases, a collective behaviour known as Franck-Condon blockade 10 . Here we show measurements on quantum dots formed in suspended single-wall carbon nanotubes revealing a remarkably large electron-vibron coupling and, due to the high quality and unprecedented tunability of our samples, admit a quantitative analysis of vibronmediated electronic transport in the regime of strong electron-vibron coupling. This allows us to unambiguously demonstrate the Franck-Condon blockade in a suspended nanostructure. The large observed electron-vibron coupling could ultimately be a key ingredient for the detection of quantized mechanical motion 11,12 . It also emphasizes the unique potential for nanoelectromechanical device applications based on suspended graphene sheets and carbon nanotubes. In a polar semiconductor, a conduction electron deforms the surrounding lattice to form a polaron state 13 . The formation of this quasi-particle, by combining an electron and a cloud of lattice vibrations, or phonons, strongly influences the transport properties. The possibility for localization of strongly coupled polarons was suggested by Landau more than 70 years ago 13 . Recently, Koch et al. predicted that a related trapping of heavy polarons can occur in a quantum dot (QD) formed in a mechanically suspended nanostructure 10 . In such a nanoelectromechanical system (NEMS), the vibrational modes of the nanostructure can be strongly affected by the presence of electrons in the QD, as they deform the embedding medium. For strong electron-phonon coupling, the deformation effectively blocks electronic transport, termed Franck-Condon (FC) blockade. By analysing electronic transport through a suspended carbon nanotube (CNT) quantum dot over a wide range of electronic states, we are able to highlight generic features of vibron-assisted electronic transport, and unambiguously confirm the FC blockade scenario.Scanning electron microscope images and a scheme of our suspended CNT quantum dot device are shown in Figs. 1a, 1b and 1c. The CNT is electrically and mechanically connected to both source (S) and drain (D) contacts, while the central electrode acts as a suspended top-gate (TG). A quantum dot in the CNT is formed between defects 14 , which are presumably created during the release process and act as local barriers. The double top-and back-gat...
Geometric symmetries cause orbital degeneracies in a molecule's spectrum. In a single-molecule junction, these degeneracies are lifted by various symmetry-breaking effects. We study quantum transport through such nanostructures with an almost degenerate spectrum. We show that the master equation for the reduced density matrix must be derived within the singular-coupling limit as opposed to the conventional weak-coupling limit. This results in strong signatures of the density matrix's off-diagonal elements in the transport characteristics.
We consider electronic transport through a single-molecule junction where the molecule has a degenerate spectrum. Unlike previous transport models, and theories a rate-equations description is no longer possible, and the quantum coherences between degenerate states have to be taken into account. We present the derivation and application of a master equation that describes the system in the weak-coupling limit and give an in-depth discussion of the parameter regimes and the new phenomena due to coherent on-site dynamics.
Rate equations are a common tool to describe the transport properties of weakly coupled single-molecule junctions. Here, we study the physics of the Anderson-Holstein model at a single vibronic resonance. We derive conditions on the Franck-Condon factors that the resonance increases or decreases the stationary current thus causing negative differential conductance. The role of backscattering of charge at vibronic resonances is also investigated. In strongly asymmetrically coupled devices backscattering causes the resonance to split into two. In symmetrically coupled devices, the Fano factor shows nonmonotonicities, which are related to correlations of forward and backward scattering of charge.
The vibrational modes of Jahn-Teller molecules are affected by a Berry phase that is associated with a conical intersection of the adiabatic potentials. We investigate theoretically how this Berry phase affects transport through a single $E \otimes e$ Jahn-Teller molecule when the tunneling electrons continually switch the molecule between a symmetric and a Jahn-Teller distorted charge state. We find that the Berry phase in conjunction with a spectral trapping mechanism leads to a current blockade even in regions outside the Coulomb blockade. The blockade is strongly asymmetric in the gate voltage and induces pronounced negative differential conductance.Comment: extended versio
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