Ab initio study of a mechanically gated molecule: From weak to strong correlation

The electronic spectrum of a chemically contacted molecule in the junction of a scanning tunneling microscope can be modified by tip retraction. We analyze this effect by a combination of density functional, many-body perturbation and numerical renormalization group theory, taking into account both the non-locality and the dynamics of electronic correlation. Our findings, in particular the evolution from a broad quasiparticle resonance below to a narrow Kondo resonance at the Fermi energy, correspond to the experimental observations.Comment: 4 pages, 3 figure

Electrical transport through a mechanically gated molecular wire

A surface-adsorbed molecule is contacted with the tip of a scanning tunneling microscope (STM) at a pre-defined atom. On tip retraction, the molecule is peeled off the surface. During this experiment, a two-dimensional differential conductance map is measured on the plane spanned by the bias voltage and the tip-surface distance. The conductance map demonstrates that tip retraction leads to mechanical gating of the molecular wire in the STM junction. The experiments are compared with a detailed ab initio simulation. We find that density functional theory (DFT) in the local density approximation (LDA) describes the tip-molecule contact formation and the geometry of the molecular junction throughout the peeling process with predictive power. However, a DFT-LDA-based transport simulation following the non-equilibrium Green's functions (NEGF) formalism fails to describe the behavior of the differential conductance as found in experiment. Further analysis reveals that this failure is due to the mean-field description of electron correlation in the local density approximation. The results presented here are expected to be of general validity and show that, for a wide range of common wire configurations, simulations which go beyond the mean-field level are required to accurately describe current conduction through molecules. Finally, the results of the present study illustrate that well-controlled experiments and concurrent ab initio transport simulations that systematically sample a large configuration space of molecule-electrode couplings allow the unambiguous identification of correlation signatures in experiment.Comment: 31 pages, 10 figure

Dynamical bi-stability of single-molecule junctions: A combined experimental/theoretical study of PTCDA on Ag(111)

The dynamics of a molecular junction consisting of a PTCDA molecule between the tip of a scanning tunneling microscope and a Ag(111) surface have been investigated experimentally and theoretically. Repeated switching of a PTCDA molecule between two conductance states is studied by low-temperature scanning tunneling microscopy for the first time, and is found to be dependent on the tip-substrate distance and the applied bias. Using a minimal model Hamiltonian approach combined with density-functional calculations, the switching is shown to be related to the scattering of electrons tunneling through the junction, which progressively excite the relevant chemical bond. Depending on the direction in which the molecule switches, different molecular orbitals are shown to dominate the transport and thus the vibrational heating process. This in turn can dramatically affect the switching rate, leading to non-monotonic behavior with respect to bias under certain conditions. In this work, rather than simply assuming a constant density of states as in previous works, it was modeled by Lorentzians. This allows for the successful description of this non-monotonic behavior of the switching rate, thus demonstrating the importance of modeling the density of states realistically.Comment: 20 pages, 6 figures, 1 tabl

Double Beta Decay: Historical Review of 75 Years of Research

Main achievements during 75 years of research on double beta decay have been reviewed. The existing experimental data have been presented and the capabilities of the next-generation detectors have been demonstrated.Comment: 25 pages, typos adde

Postdeposition annealing induced transition from hexagonal Pr2O3Pr_2O_3 to cubic PrO2PrO_2 films on Si(111)

Films of hexagonal praseodymium sesquioxide (h-Pr$_2$O$_3$) were deposited on Si(111) by molecular beam epitaxy and thereafter annealed in 1 atm oxygen at different temperatures, ranging from 100 to 700 °C. The films of the samples annealed at 300 °C or more were transformed to PrO2 with B-oriented Fmˉ3m structure, while films annealed at lower temperatures kept the hexagonal structure. The films are composed of PrO2 and PrO2−δ species, which coexist laterally and are tetragonally distorted due to the interaction at the interface between oxide film and Si substrate. Compared to PrO$_2$, PrO$_2$−δ has the same cubic structure but with oxygen vacancies. The oxygen vacancies are partly ordered and increase the vertical lattice constant of the film, whereas the lateral lattice constant is almost identical for both species and on all samples. The latter lattice constant matches the lattice constant of the originally crystallized hexagonal praseodymium sesquioxide. That means that no long range reordering of the praseodymium atoms takes place during the phase transformatio

Effect of Amorphous Interface Layers on Crystalline Thin-Film X-Ray Diffraction

In this work, an analysis method of x-ray diffraction data of crystalline structures with amorphous interface layers is presented and applied to single crystalline films on amorphous interface layers. Thickness and morphology of crystalline films are obtained from x-ray diffraction at conditions where no significant interference effects between crystalline film and substrate occur. Extending the x-ray diffraction analysis to conditions where interference effects between the crystalline film and the substrate appear, it is also possible to determine the morphology of the amorphous interface film. The analysis method presented in this work is useful for the current and future analyses of amorphous structures between crystalline structures in general and is therefore applicable to many different material systems. This incorporates crystalline thin and ultrathin films on crystalline substrates as well as crystalline multilayers on crystalline and also on amorphous substrates. We apply the method developed here to characterize both crystalline praseodymia films and amorphous interface layers, which could be detected neither by x-ray reflection nor by x-ray diffraction previously