arXiv subjects

Herre S. J. van der Zant

Publications and source records attributed to Herre S. J. van der Zant.

150 records · Page 9Linked to original sources

arXiv2010

Vibrational Excitations in Weakly Coupled Single-Molecule Junctions: A Computational Analysis

In bulk systems, molecules are routinely identified by their vibrational spectrum using Raman or infrared spectroscopy. In recent years, vibrational excitation lines have been observed in low-temperature conductance measurements on single molecule junctions and they can provide a similar means of identification. We present a method to efficiently calculate these excitation lines in weakly coupled, gateable single-molecule junctions, using a combination of ab initio density functional theory and rate equations. Our method takes transitions from excited to excited vibrational state into account by evaluating the Franck-Condon factors for an arbitrary number of vibrational quanta, and is therefore able to predict qualitatively different behaviour from calculations limited to transitions from ground state to excited vibrational state. We find that the vibrational spectrum is sensitive to the molecular contact geometry and the charge state, and that it is generally necessary to take more than one vibrational quantum into account. Quantitative comparison to previously reported measurements on pi-conjugated molecules reveals that our method is able to characterize the vibrational excitations and can be used to identify single molecules in a junction. The method is computationally feasible on commodity hardware.

cond-mat.mes-hall↗

arXiv2009

Electrical manipulation of spin states in a single electrostatically gated transition-metal complex

We demonstrate an electrically controlled high-spin (S=5/2) to low-spin (S=1/2) transition in a three-terminal device incorporating a single Mn2+ ion coordinated by two terpyridine ligands. By adjusting the gate-voltage we reduce the terpyridine moiety and thereby strengthen the ligand-field on the Mn-atom. Adding a single electron thus stabilizes the low-spin configuration and the corresponding sequential tunnelling current is suppressed by spin-blockade. From low-temperature inelastic cotunneling spectroscopy, we infer the magnetic excitation spectrum of the molecule and uncover also a strongly gate-dependent singlet-triplet splitting on the low-spin side. The measured bias-spectroscopy is shown to be consistent with an exact diagonalization of the Mn-complex, and an interpretation of the data is given in terms of a simplified effective model.

cond-mat.mes-hall↗

arXiv2008

Nanomechanical properties of few-layer graphene membranes

We have measured the mechanical properties of few-layer graphene and graphite flakes that are suspended over circular holes. The spatial profile of the flake's spring constant is measured with an atomic force microscope. The bending rigidity of and the tension in the membranes are extracted by fitting a continuum model to the data. For flakes down to eight graphene layers, both parameters show a strong thickness-dependence. We predict fundamental resonance frequencies of these nanodrums in the GHz range based on the measured bending rigidity and tension.

cond-mat.mes-hall↗

arXiv2007

Electronic excitations of a single molecule contacted in a three-terminal configuration

Low-temperature three-terminal transport measurements through a thiol end-capped Pi -conjugated molecule have been carried out. Electronic excitations, including zero and finite-bias Kondo-effects have been observed and studied as a function of magnetic field. Using a simplified two-orbital model we have accounted for the spin and the electronic configuration of the first four charge states of the molecule. The charge-dependent couplings to gate, source and drain electrodes suggest a scenario in which charges and spins are localized at the ends of the molecule, close to the electrodes.

cond-mat.mes-hall↗

arXiv2005

Orbital Kondo effect in carbon nanotubes

Progress in the fabrication of nanometer-scale electronic devices is opening new opportunities to uncover the deepest aspects of the Kondo effect, one of the paradigmatic phenomena in the physics of strongly correlated electrons. Artificial single-impurity Kondo systems have been realized in various nanostructures, including semiconductor quantum dots, carbon nanotubes and individual molecules. The Kondo effect is usually regarded as a spin-related phenomenon, namely the coherent exchange of the spin between a localized state and a Fermi sea of electrons. In principle, however, the role of the spin could be replaced by other degrees of freedom, such as an orbital quantum number. Here we demonstrate that the unique electronic structure of carbon nanotubes enables the observation of a purely orbital Kondo effect. We use a magnetic field to tune spin-polarized states into orbital degeneracy and conclude that the orbital quantum number is conserved during tunneling. When orbital and spin degeneracies are simultaneously present, we observe a strongly enhanced Kondo effect, with a multiple splitting of the Kondo resonance at finite field and predicted to obey a so-called SU(4) symmetry.

cond-mat.mes-hall↗

arXiv2004

Electron-hole symmetry in a semiconducting carbon nanotube quantum dot

Optical and electronic phenomena in solids arise from the behaviour of electrons and holes (unoccupied states in a filled electron sea). Electron-hole symmetry can often be invoked as a simplifying description, which states that electrons with energy above the Fermi sea behave the same as holes below the Fermi energy. In semiconductors, however, electron-hole symmetry is generally absent since the energy band structure of the conduction band differs from the valence band. Here we report on measurements of the discrete, quantized-energy spectrum of electrons and holes in a semiconducting carbon nanotube. Through a gate, an individual nanotube is filled controllably with a precise number of either electrons or holes, starting from one. The discrete excitation spectrum for a nanotube with N holes is strikingly similar to the corresponding spectrum for N electrons. This observation of near perfect electron-hole symmetry demonstrates for the first time that a semiconducting nanotube can be free of charged impurities, even in the limit of few-electrons or holes. We furthermore find an anomalously small Zeeman spin splitting and an excitation spectrum indicating strong electron-electron interactions.

cond-mat.mes-hall↗