Counting statistics of tunneling through a single molecule: effect of distortion and displacement of vibrational potential surface

We analyze the effects of a distortion of the nuclear potential of a molecular quantum dot (QD), as well as a shift of its equilibrium position, on nonequilibrium-vibration-assisted tunneling through the QD with a single level ($\epsilon_d$) coupled to the vibrational mode. For this purpose, we derive an explicit analytical expression for the Franck-Condon (FC) factor for a displaced-distorted oscillator surface of the molecule and establish rate equations in the joint electron-phonon representation to examine the current-voltage characteristics and zero-frequency shot noise, and skewness as well. Our numerical analyses shows that the distortion has two important effects. The first one is that it breaks the symmetry between the excitation spectra of the charge states, leading to asymmetric tunneling properties with respect to $\epsilon_d>0$ and $\epsilon_d<0$. Secondly, distortion (frequency change of the oscillator) significantly changes the voltage-activated cascaded transition mechanism, and consequently gives rise to a different nonequilibrium vibrational distribution from that of the case without distortion. Taken in conjunction with strongly modified FC factors due to distortion, this results in some new transport features: the appearance of strong NDC even for a single-level QD with symmetric tunnel couplings; a giant Fano factor even for a molecule with an extremely weak electron-phonon interaction; and enhanced skewness that can have a large negative value under certain conditions.Comment: 29 pages, 11 figures, published versio

Excitation and emission spectra of rubidium in rare-gas thin-films

To understand the optical properties of atoms in solid state matrices, the absorption, excitation and emission spectra of rubidium doped thin-films of argon, krypton and xenon were investigated in detail. A two-dimensional spectral analysis extends earlier reports on the excitation and emission properties of rubidium in rare-gas hosts. We found that the doped crystals of krypton and xenon exhibit a simple absorption-emission relation, whereas rubidium in argon showed more complicated spectral structures. Our sample preparation employed in the present work yielded different results for the Ar crystal, but our peak positions were consistent with the prediction based on the linear extrapolation of Xe and Kr data. We also observed a bleaching behavior in rubidium excitation spectra, which suggests a population transfer from one to another spectral feature due to hole-burning. The observed optical response implies that rubidium in rare-gas thin-films is detectable with extremely high sensitivity, possibly down to a single atom level, in low concentration samples.Comment: 7 pages, 5 figure

Non-adiabatic Effects in the Dissociation of Oxygen Molecules at the Al(111) Surface

The measured low initial sticking probability of oxygen molecules at the Al(111) surface that had puzzled the field for many years was recently explained in a non-adiabatic picture invoking spin-selection rules [J. Behler et al., Phys. Rev. Lett. 94, 036104 (2005)]. These selection rules tend to conserve the initial spin-triplet character of the free O2 molecule during the molecule's approach to the surface. A new locally-constrained density-functional theory approach gave access to the corresponding potential-energy surface (PES) seen by such an impinging spin-triplet molecule and indicated barriers to dissociation which reduce the sticking probability. Here, we further substantiate this non-adiabatic picture by providing a detailed account of the employed approach. Building on the previous work, we focus in particular on inaccuracies in present-day exchange-correlation functionals. Our analysis shows that small quantitative differences in the spin-triplet constrained PES obtained with different gradient-corrected functionals have a noticeable effect on the lowest kinetic energy part of the resulting sticking curve.Comment: 17 pages including 11 figures; related publications can be found at http://www.fhi-berlin.mpg.de/th/th.htm

A formal model of the Document Object Model

This is the final version. Available from AFP via the link in this recordIn this AFP entry, we formalize the core of the Document Object Model (DOM). At its core, the DOM defines a tree-like data structure for representing documents in general and HTML documents in particular. It is the heart of any modern web browser. Formalizing the key concepts of the DOM is a prerequisite for the formal reasoning over client-side JavaScript programs and for the analysis of security concepts in modern web browsers. We present a formalization of the core DOM, with focus on the node-tree and the operations defined on node-trees, in Isabelle/HOL. We use the formalization to verify the functional correctness of the most important functions defined in the DOM standard. Moreover, our formalization is 1) extensible, i.e., can be extended without the need of re-proving already proven properties and 2) executable, i.e., we can generate executable code from our specification

Predicting and verifying transition strengths from weakly bound molecules

We investigated transition strengths from ultracold weakly bound 41K87Rb molecules produced via the photoassociation of laser-cooled atoms. An accurate potential energy curve of the excited state (3)1Sigma+ was constructed by carrying out direct potential fit analysis of rotational spectra obtained via depletion spectroscopy. Vibrational energies and rotational constants extracted from the depletion spectra of v'=41-50 levels were combined with the results of the previous spectroscopic study, and they were used for modifying an ab initio potential. An accuracy of 0.14% in vibrational level spacing and 0.3% in rotational constants was sufficient to predict the large observed variation in transition strengths among the vibrational levels. Our results show that transition strengths from weakly bound molecules are a good measure of the accuracy of an excited state potential.Comment: 7 pages, 7 figure

Quantum initial condition sampling for linearized density matrix dynamics: Vibrational pure dephasing of iodine in krypton matrices

This paper reviews the linearized path integral approach for computing time dependent properties of systems that can be approximated using a mixed quantum-classical description. This approach is applied to studying vibrational pure dephasing of ground state molecular iodine in a rare gas matrix. The Feynman-Kleinert optimized harmonic approximation for the full system density operator is used to sample initial conditions for the bath degrees of freedom. This extremely efficient approach is compared with alternative initial condition sampling techniques at low temperatures where classical initial condition sampling yields dephasing rates that are nearly an order of magnitude too slow compared with quantum initial condition sampling and experimental results.Comment: 20 pages and 8 figure

CO oxidation at Pd(100): A first-principles constrained thermodynamics study

The possible formation of oxides or thin oxide films (surface oxides) on late transition metal surfaces is recently being recognized as an essential ingredient when aiming to understand catalytic oxidation reactions under technologically relevant gas phase conditions. Using the CO oxidation at Pd(100) as example, we investigate the composition and structure of this model catalyst surface over a wide range of (T,p)-conditions within a multiscale modeling approach where density-functional theory is linked to thermodynamics. The results show that under the catalytically most relevant gas phase conditions a thin surface oxide is the most stable "phase" and that the system is actually very close to a transition between this oxidic state and a reduced state in form of a CO covered Pd(100) surface.Comment: 13 pages including 7 figures; related publications can be found at http://www.fhi-berlin.mpg.de/th/th.htm

Controlled Production of Sub-Radiant States of a Diatomic Molecule in an Optical Lattice

We report successful production of sub-radiant states of a two-atom system in a three-dimensional optical lattice starting from doubly occupied sites in a Mott insulator phase of a quantum gas of atomic ytterbium. We can selectively produce either sub-radiant 1g state or super-radiant 0u state by choosing the excitation laser frequency. The inherent weak excitation rate for the sub-radiant 1g state is overcome by the increased atomic density due to the tight-confinement in a three-dimensional optical lattice. Our experimental measurements of binding energies, linewidth, and Zeeman shift confirm observation of sub-radiant levels of the 1g state of the Yb_2 molecule.Comment: To be published in Phys. Rev. Let

On the mutual polarization of two He-4 atoms

We propose a simple method based on the standard quantum-mechanical perturbation theory to calculate the mutual polarization of two atoms He^4.Comment: 9 pages, 1 table; the article is revised and the calculation is essentially refined; v4: final version, the Introduction is delete