Theoretical study of the charge transport through C60-based single-molecule junctions

We present a theoretical study of the conductance and thermopower of single-molecule junctions based on C60 and C60-terminated molecules. We first analyze the transport properties of gold-C60-gold junctions and show that these junctions can be highly conductive (with conductances above 0.1G0, where G0 is the quantum of conductance). Moreover, we find that the thermopower in these junctions is negative due to the fact that the LUMO dominates the charge transport, and its magnitude can reach several tens of micro-V/K, depending on the contact geometry. On the other hand, we study the suitability of C60 as an anchoring group in single-molecule junctions. For this purpose, we analyze the transport through several dumbbell derivatives using C60 as anchors, and we compare the results with those obtained with thiol and amine groups. Our results show that the conductance of C60-terminated molecules is rather sensitive to the binding geometry. Moreover, the conductance of the molecules is typically reduced by the presence of the C60 anchors, which in turn makes the junctions more sensitive to the functionalization of the molecular core with appropriate side groups.Comment: 9 pages, 7 figure

Tuning the thermal conductance of molecular junctions with interference effects

We present an \emph{ab initio} study of the role of interference effects in the thermal conductance of single-molecule junctions. To be precise, using a first-principles transport method based on density functional theory, we analyze the coherent phonon transport in single-molecule junctions based on several benzene and oligo-phenylene-ethynylene derivatives. We show that the thermal conductance of these junctions can be tuned via the inclusion of substituents, which induces destructive interference effects and results in a decrease of the thermal conductance with respect to the unmodified molecules. In particular, we demonstrate that these interference effects manifest as antiresonances in the phonon transmission, whose energy positions can be controlled by varying the mass of the substituents. Our work provides clear strategies for the heat management in molecular junctions and more generally in nanostructured metal-organic hybrid systems, which are important to determine, how these systems can function as efficient energy-conversion devices such as thermoelectric generators and refrigerators

Field enhancement in subnanometer metallic gaps

Motivated by recent experiments [Ward et al., Nature Nanotech. 5, 732 (2010)], we present here a theoretical analysis of the optical response of sharp gold electrodes separated by a subnanometer gap. In particular, we have used classical finite difference time domain simulations to investigate the electric field distribution in these nanojunctions upon illumination. Our results show a strong confinement of the field within the gap region, resulting in a large enhancement compared to the incident field. Enhancement factors exceeding 1000 are found for interelectrode distances on the order of a few angstroms, which are fully compatible with the experimental findings. Such huge enhancements originate from the coupling of the incident light to the evanescent field of hybrid plasmons involving charge density oscillations in both electrodes.Comment: 4 pages, 3 figures, to appear in Physical Review

Chemical Bonding and Charge Distribution at Metallic Nanocontacts

We present results of electronic structure calculations for aluminium contacts of atomic size, based on density functional theory and the local density approximation. Addressing the atomic orbitals at the neck of the nanocontact, we find that the local band structure deviates strongly from bulk fcc aluminium. In particular, hybridization between Al 3s and 3p states is fully suppressed due to directed bonds at the contact. Moreover, a charge transfer of 0.6 electrons off the contact aluminium site is found. Both the suppressed hybridization and the violated charge neutrality are characteristic features of metallic nanocontacts. This fact has serious consequences for models aiming at a microscopic description of transport properties.Comment: 6 pages, 3 figures, accepted by Chemical Physics Letter

Thresholds for breather solutions on the Discrete Nonlinear Schr\"odinger Equation with saturable and power nonlinearity

We consider the question of existence of periodic solutions (called breather solutions or discrete solitons) for the Discrete Nonlinear Schr\"odinger Equation with saturable and power nonlinearity. Theoretical and numerical results are proved concerning the existence and nonexistence of periodic solutions by a variational approach and a fixed point argument. In the variational approach we are restricted to DNLS lattices with Dirichlet boundary conditions. It is proved that there exists parameters (frequency or nonlinearity parameters) for which the corresponding minimizers satisfy explicit upper and lower bounds on the power. The numerical studies performed indicate that these bounds behave as thresholds for the existence of periodic solutions. The fixed point method considers the case of infinite lattices. Through this method, the existence of a threshold is proved in the case of saturable nonlinearity and an explicit theoretical estimate which is independent on the dimension is given. The numerical studies, testing the efficiency of the bounds derived by both methods, demonstrate that these thresholds are quite sharp estimates of a threshold value on the power needed for the the existence of a breather solution. This it justified by the consideration of limiting cases with respect to the size of the nonlinearity parameters and nonlinearity exponents.Comment: 26 pages, 10 figure

Interplay Between Yu-Shiba-Rusinov States and Multiple Andreev Reflections

Motivated by recent scanning tunneling microscopy experiments on single magnetic impurities on superconducting surfaces, we present here a comprehensive theoretical study of the interplay between Yu-Shiba-Rusinov bound states and (multiple) Andreev reflections. Our theory is based on a combination of an Anderson model with broken spin degeneracy and nonequilibrium Green's function techniques that allows us to describe the electronic transport through a magnetic impurity coupled to superconducting leads for arbitrary junction transparency. Using this combination we are able to elucidate the different tunneling processes that give a significant contribution to the subgap transport. In particular, we predict the occurrence of a large variety of Andreev reflections mediated by Yu-Shiba-Rusinov bound states that clearly differ from the standard Andreev processes in non-magnetic systems. Moreover, we provide concrete guidelines on how to experimentally identify the subgap features originating from these tunneling events. Overall, our work provides new insight into the role of the spin degree of freedom in Andreev transport physics.Comment: 15 pages, 10 figure

Critical generalized inverse participation ratio distributions

The system size dependence of the fluctuations in generalized inverse participation ratios (IPR's) $I_{\alpha}(q)$ at criticality is investigated numerically. The variances of the IPR logarithms are found to be scale-invariant at the macroscopic limit. The finite size corrections to the variances decay algebraically with nontrivial exponents, which depend on the Hamiltonian symmetry and the dimensionality. The large-$q$ dependence of the asymptotic values of the variances behaves as $q^2$ according to theoretical estimates. These results ensure the self-averaging of the corresponding generalized dimensions.Comment: RevTex4, 5 pages, 4 .eps figures, to be published in Phys. Rev.

Extraordinary transverse magneto-optical Kerr effect in a superlens

It has been shown that a slab of a negative index material can behave as a superlens enhancing the imaging resolution beyond the wavelength limit. We show here that if such a slab possesses in addition some magneto-optical activity, it could act as an ideal optical filter and exhibit an extraordinary transverse magneto-optical Kerr effect. Moreover, we show that losses, which spoil the imaging resolution of these lenses, are a necessary ingredient to observe this effect.Comment: 5 pages, 6 figure

Vibrational Instabilities in Resonant Electron Transport through Single-Molecule Junctions

We analyze various limits of vibrationally coupled resonant electron transport in single-molecule junctions. Based on a master equation approach, we discuss analytic and numerical results for junctions under a high bias voltage or weak electronic-vibrational coupling. It is shown that in these limits the vibrational excitation of the molecular bridge increases indefinitely, i.e. the junction exhibits a vibrational instability. Moreover, our analysis provides analytic results for the vibrational distribution function and reveals that these vibrational instabilities are related to electron-hole pair creation processes.Comment: 19 pages, 3 figure