Image effects in transport at metal-molecule interfaces

We present a method for incorporating image-charge effects into the description of charge transport through molecular devices. A simple model allows us to calculate the adjustment of the transport levels, due to the polarization of the electrodes as charge is added to and removed from the molecule. For this, we use the charge distributions of the molecule between two metal electrodes in several charge states, rather than in gas phase, as obtained from a density-functional theory-based transport code. This enables us to efficiently model level shifts and gap renormalization caused by image-charge effects, which are essential for understanding molecular transport experiments. We apply the method to benzene di-amine molecules and compare our results with the standard approach based on gas phase charges. Finally, we give a detailed account of the application of our approach to porphyrin-derivative devices recently studied experimentally by Perrin et al. [Nat. Nanotechnol. 8, 282 (2013)], which demonstrates the importance of accounting for image-charge effects when modeling transport through molecular junctions

Evidence for LineLike Vortex Liquid Phase in Tl2_2Ba2_2CaCu2_2O8_8 Probed by the Josephson Plasma Resonance

We measured the Josephson plasma resonance (JPR) in optimally doped Tl$_2$Ba$_2$CaCu$_2$O$_{8+\delta}$ thin films using terahertz time-domain spectroscopy in transmission. The temperature and magnetic field dependence of the JPR frequency shows that the c-axis correlations of pancake vortices remain intact at the transition from the vortex solid to the liquid phase. In this respect Tl$_2$Ba$_2$CaCu$_2$O$_{8+\delta}$ films, withanisotropy parameter $\gamma\approx 150$, are similar to the less anisotropic YBa$_2$Cu$_3$O$_{7-\delta}$ $(\gamma\approx 8)$ rather than to the most anisotropic Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ single crystals $\gamma\geq 500$).Comment: Submitted to Physical Review Letter

Transverse optical Josephson plasmons, equations of motion

A detailed calculation is presented of the dielectric function in superconducttors consisting of two Josephson coupled superconducting layers per unit cell, taking into account the effect of finite compressibility of the electron fluid. From the model it follows, that two longitudinal, and one transverse optical Josephson plasma resonance exist in these materials, for electric field polarization perpendicular to the planes. The latter mode appears as a resonance in the transverse dielectric function, and it couples directly to the electrical field vector of infrared radiation. A shift of all plasma frequencies, and a reduction of the intensity of the transverse optical Josephson plasmon is shown to result from the finite compressibility of the electron fluid.Comment: 17 pages, ReVTeX, 7 figures in eps forma

Large tunable image-charge effects in single-molecule junctions

The characteristics of molecular electronic devices are critically determined by metal-organic interfaces, which influence the arrangement of the orbital levels that participate in charge transport. Studies on self-assembled monolayers (SAMs) show (molecule-dependent) level shifts as well as transport-gap renormalization, suggesting that polarization effects in the metal substrate play a key role in the level alignment with respect to the metal's Fermi energy. Here, we provide direct evidence for an electrode-induced gap renormalization in single-molecule junctions. We study charge transport in single porphyrin-type molecules using electrically gateable break junctions. In this set-up, the position of the occupied and unoccupied levels can be followed in situ and with simultaneous mechanical control. When increasing the electrode separation, we observe a substantial increase in the transport gap with level shifts as high as several hundreds of meV for displacements of a few \aa ngstroms. Analysis of this large and tunable gap renormalization with image-charge calculations based on atomic charges obtained from density functional theory confirms and clarifies the dominant role of image-charge effects in single-molecule junctions

Unravelling the conductance path through single-porphyrin junctions

Porphyrin derivatives are key components in natural machinery enabling us to store sunlight as chemical energy. In spite of their prominent role in cascades separating electrical charges and their potential as sensitizers in molecular devices, reports concerning their electronic transport characteristics are inconsistent. Here we report a systematic investigation of electronic transport paths through single porphyrin junctions. The transport through seven structurally related porphyrin derivatives was repeatedly measured in an automatized mechanically controlled break-junction set-up and the recorded data were analyzed by an unsupervised clustering algorithm. The correlation between the appearances of similar clusters in particular sub-sets of the porphyrins with a common structural motif allowed us to assign the corresponding current path. The small series of model porphyrins allowed us to identify and distinguish three different electronic paths covering more than four orders of magnitude in conductance

Field Dependence of the Josephson Plasma Resonance in Layered Superconductors with Alternating Junctions

The Josephson plasma resonance in layered superconductors with alternating critical current densities is investigated in a low perpendicular magnetic field. In the vortex solid phase the current densities and the squared bare plasma frequencies decrease linearly with the magnetic field. Taking into account the coupling due to charge fluctuations on the layers, we extract from recent optical data for SmLa_{1-x} Sr_x CuO_{4-delta} the Josephson penetration length lambda_{ab} approximately 1100 A parallel to the layers at T=10 K.Comment: 5 pages, 6 eps-figures, final version with minor misprints correcte

Interlayer pair tunneling and gap anisotropy in YBa2_2Cu3_3O7−δ_{7-\delta}

Recent ARPES measurement observed a large $ab$-axis gap anisotropy, $\Delta(0,\pi)/\Delta(\pi,0)=1.5$, in clean YBa$_2$Cu$_3$O$_{7-\delta}$. This indicates that some sub-dominant component may exist in the $d_{x^2-y^2}$-wave dominant gap. We propose that the interlayer pairing tunneling contribution can be determined through the investigation of the order parameter anisotropy. Their potentially observable features in transport and spin dynamics are also studied.Comment: 4 pages, 3 figure

Observation of the Transverse Optical Plasmon in SmLa0.8Sr0.2CuO4-d

We present microwave and infrared measurements on SmLa0.8Sr0.2CuO4-d, which are direct evidence for the existence of a transverse optical plasma mode, observed as a peak in the c-axis optical conductivity. This mode appears as a consequence of the existence of two different intrinsic Josephson couplings between the CuO2 layers, one with a Sm2O2 block layer, and the other one with a (La,Sr)O block layer. From the frequencies and the intensities of the collective modes we determine the value of the compressibility of the two dimensional electron fluid in the copper oxygen planes.Comment: REVTeX, 4 pages, 5 eps-figures, PRL, in pres