Non-Adiabatic Potential-Energy Surfaces by Constrained Density-Functional Theory

Non-adiabatic effects play an important role in many chemical processes. In order to study the underlying non-adiabatic potential-energy surfaces (PESs), we present a locally-constrained density-functional theory approach, which enables us to confine electrons to sub-spaces of the Hilbert space, e.g. to selected atoms or groups of atoms. This allows to calculate non-adiabatic PESs for defined charge and spin states of the chosen subsystems. The capability of the method is demonstrated by calculating non-adiabatic PESs for the scattering of a sodium and a chlorine atom, for the interaction of a chlorine molecule with a small metal cluster, and for the dissociation of an oxygen molecule at the Al(111) surface.Comment: 11 pages including 7 figures; related publications can be found at http://www.fhi-berlin.mpg.de/th/th.htm

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

Coulomb Gap and Correlated Vortex Pinning in Superconductors

The positions of columnar pins and magnetic flux lines determined from a decoration experiment on BSCCO were used to calculate the single--particle density of states at low temperatures in the Bose glass phase. A wide Coulomb gap is found, with gap exponent $s \approx 1.2$, as a result of the long--range interaction between the vortices. As a consequence, the variable--range hopping transport of flux lines is considerably reduced with respect to the non--interacting case, the effective Mott exponent being enhanced from $p_0 = 1/3$ to $p_{\rm eff} \approx 0.5$ for this specific experiment.Comment: 10 pages, Revtex, 4 figures appended as uu-encoded postscript files, also available as hardcopies from [email protected]

Atomic-scale representation and statistical learning of tensorial properties

This chapter discusses the importance of incorporating three-dimensional symmetries in the context of statistical learning models geared towards the interpolation of the tensorial properties of atomic-scale structures. We focus on Gaussian process regression, and in particular on the construction of structural representations, and the associated kernel functions, that are endowed with the geometric covariance properties compatible with those of the learning targets. We summarize the general formulation of such a symmetry-adapted Gaussian process regression model, and how it can be implemented based on a scheme that generalizes the popular smooth overlap of atomic positions representation. We give examples of the performance of this framework when learning the polarizability and the ground-state electron density of a molecule

Measurement of the branching ratio of the decay Ξ0→Σ+μ−νˉμ\Xi^{0}\rightarrow \Sigma^{+} \mu^{-} \bar{\nu}_{\mu}

From the 2002 data taking with a neutral kaon beam extracted from the CERN-SPS, the NA48/1 experiment observed 97 $\Xi^{0}\rightarrow \Sigma^{+} \mu^{-} \bar{\nu}_{\mu}$ candidates with a background contamination of $30.8 \pm 4.2$ events. From this sample, the BR($\Xi^{0}\rightarrow \Sigma^{+} \mu^{-} \bar{\nu}_{\mu}$) is measured to be $(2.17 \pm 0.32_{\mathrm{stat}}\pm 0.17_{\mathrm{syst}})\times10^{-6}$

Do columnar defects produce bulk pinning?

From magneto-optical imaging performed on heavy-ion irradiated YBaCuO single crystals, it is found that at fields and temperatures where strong single vortex pinning by individual irradiation-induced amorphous columnar defects is to be expected, vortex motion is limited by the nucleation of vortex kinks at the specimen surface rather than by half-loop nucleation in the bulk. In the material bulk, vortex motion occurs through (easy) kink sliding. Depinning in the bulk determines the screening current only at fields comparable to or larger than the matching field, at which the majority of moving vortices is not trapped by an ion track.Comment: 5 pages, 5 figures, submitted to Physical Review Letter

Building nonparametric nn-body force fields using Gaussian process regression

Constructing a classical potential suited to simulate a given atomic system is a remarkably difficult task. This chapter presents a framework under which this problem can be tackled, based on the Bayesian construction of nonparametric force fields of a given order using Gaussian process (GP) priors. The formalism of GP regression is first reviewed, particularly in relation to its application in learning local atomic energies and forces. For accurate regression it is fundamental to incorporate prior knowledge into the GP kernel function. To this end, this chapter details how properties of smoothness, invariance and interaction order of a force field can be encoded into corresponding kernel properties. A range of kernels is then proposed, possessing all the required properties and an adjustable parameter $n$ governing the interaction order modelled. The order $n$ best suited to describe a given system can be found automatically within the Bayesian framework by maximisation of the marginal likelihood. The procedure is first tested on a toy model of known interaction and later applied to two real materials described at the DFT level of accuracy. The models automatically selected for the two materials were found to be in agreement with physical intuition. More in general, it was found that lower order (simpler) models should be chosen when the data are not sufficient to resolve more complex interactions. Low $n$ GPs can be further sped up by orders of magnitude by constructing the corresponding tabulated force field, here named "MFF".Comment: 31 pages, 11 figures, book chapte

Recent NA48/2 and NA62 results

The NA48/2 Collaboration at CERN has accumulated and analysed unprecedented statistics of rare kaon decays in the $K_{e4}$ modes: $K_{e4}(+-)$ ($K^\pm \to \pi^+ \pi^- e^\pm \nu$) and $K_{e4}(00)$ ($K^\pm \to \pi^0 \pi^0 e^\pm \nu$) with nearly one percent background contamination. It leads to the improved measurement of branching fractions and detailed form factor studies. New final results from the analysis of 381 $K^\pm \to \pi^\pm \gamma \gamma$ rare decay candidates collected by the NA48/2 and NA62 experiments at CERN are presented. The results include a decay rate measurement and fits to Chiral Perturbation Theory (ChPT) description.Comment: Prepared for the Proceedings of "Moriond QCD and High Energy Interactions. March 22-29 2014." conferenc

Interactions, Distribution of Pinning Energies, and Transport in the Bose Glass Phase of Vortices in Superconductors

We study the ground state and low energy excitations of vortices pinned to columnar defects in superconductors, taking into account the long--range interaction between the fluxons. We consider the ``underfilled'' situation in the Bose glass phase, where each flux line is attached to one of the defects, while some pins remain unoccupied. By exploiting an analogy with disordered semiconductors, we calculate the spatial configurations in the ground state, as well as the distribution of pinning energies, using a zero--temperature Monte Carlo algorithm minimizing the total energy with respect to all possible one--vortex transfers. Intervortex repulsion leads to strong correlations whenever the London penetration depth exceeds the fluxon spacing. A pronounced peak appears in the static structure factor $S(q)$ for low filling fractions $f \leq 0.3$. Interactions lead to a broad Coulomb gap in the distribution of pinning energies $g(\epsilon)$ near the chemical potential $\mu$, separating the occupied and empty pins. The vanishing of $g(\epsilon)$ at $\mu$ leads to a considerable reduction of variable--range hopping vortex transport by correlated flux line pinning.Comment: 16 pages (twocolumn), revtex, 16 figures not appended, please contact [email protected]