Parallel and anti-parallel echoes in beam spin echo experiments

The refocusing of velocity-dependent spin-phase is the basic phenomenon behind helium and neutron spin echo beam experiments. In this paper we present quantum and classical descriptions of the spin echo phenomenon and show that non-adiabatic transitions, such as those which take place during rotation of the magnetic field axis between the two arms of a helium spin echo setup, lead to echo conditions without reversing the magnetic field orientation between the two arms. The usual spin echo conditions, created by reversing the magnetic field orientation, do not require such non-adiabatic transitions. These two echo conditions are termed parallel and anti-parallel spin echoes, respectively. We derive the dependence of the relative intensity of the two echoes on the scattering geometry of the setup and show experimental results which verify the co-existence of the two echo conditions, the theoretically derived expressions for their relative intensity and the effect of an additional spin rotator coil introduced within the non-adiabatic transition region

How Atomic Steps Modify Diffusion and Inter-adsorbate Forces: Empirical Evidence from Hopping Dynamics in Na/Cu(115).

We followed the collective atomic-scale motion of Na atoms on a vicinal Cu(115) surface within a time scale of pico- to nanoseconds using helium spin echo spectroscopy. The well-defined stepped structure of Cu(115) allows us to study the effect that atomic steps have on the adsorption properties, the rate for motion parallel and perpendicular to the step edge, and the interaction between the Na atoms. With the support of a molecular dynamics simulation we show that the Na atoms perform strongly anisotropic 1D hopping motion parallel to the step edges. Furthermore, we observe that the spatial and temporal correlations between the Na atoms that lead to collective motion are also anisotropic, suggesting the steps efficiently screen the lateral interaction between Na atoms residing on different terraces.This work was supported by the German-Israeli Foundation for Scientific Research and Development, the Israeli Science Foundation (Grant No. 2011185), the German Science Foundation (DFG) through contract MO 960/18-1, the Cluster of Excellence RESOLV (EXC 1069), and the European Research Council under the European Union’s seventh framework program (FP/2007-2013)/ERC Grant 307267.This is the author accepted manuscript. The final version is available from ACS via http://dx.doi.org/10.1021/acs.jpclett.5b0193

Two-Dimensional Wetting of a Stepped Copper Surface.

Highly corrugated, stepped surfaces present regular 1D arrays of binding sites, creating a complex, heterogeneous environment to water. Rather than decorating the hydrophilic step sites to form 1D chains, water on stepped Cu(511) forms an extended 2D network that binds strongly to the steps but bridges across the intervening hydrophobic Cu(100) terraces. The hydrogen-bonded network contains pentamer, hexamer, and octomer water rings that leave a third of the stable Cu step sites unoccupied in order to bind water H down close to the step dipole and complete three hydrogen bonds per molecule.Herchel Smith fun

Setting benchmarks for modelling gas–surface interactions using coherent control of rotational orientation states

A fundamental and predictive understanding of molecule-surface interactions is challenging to obtain. Here the authors report an experimental technique allowing direct measurement of the scattering matrix, which reports on the coherent evolution of quantum states of a molecule scattering from a surface

Let’s not forget tautomers

A compound exhibits tautomerism if it can be represented by two structures that are related by an intramolecular movement of hydrogen from one atom to another. The different tautomers of a molecule usually have different molecular fingerprints, hydrophobicities and pKa’s as well as different 3D shape and electrostatic properties; additionally, proteins frequently preferentially bind a tautomer that is present in low abundance in water. As a result, the proper treatment of molecules that can tautomerize, ~25% of a database, is a challenge for every aspect of computer-aided molecular design. Library design that focuses on molecular similarity or diversity might inadvertently include similar molecules that happen to be encoded as different tautomers. Physical property measurements might not establish the properties of individual tautomers with the result that algorithms based on these measurements may be less accurate for molecules that can tautomerize—this problem influences the accuracy of filtering for library design and also traditional QSAR. Any 2D or 3D QSAR analysis must involve the decision of if or how to adjust the observed Ki or IC50 for the tautomerization equilibria. QSARs and recursive partitioning methods also involve the decision as to which tautomer(s) to use to calculate the molecular descriptors. Docking virtual screening must involve the decision as to which tautomers to include in the docking and how to account for tautomerization in the scoring. All of these decisions are more difficult because there is no extensive database of measured tautomeric ratios in both water and non-aqueous solvents and there is no consensus as to the best computational method to calculate tautomeric ratios in different environments