Sequential homobimetallic catalysis: an unprecedented tandem Pd(0)-catalysed deprotection - Pd(II)-catalysed heterocyclisation reaction leading to benzofurans

We report here the first example of "sequential homobimetallic catalysis": a transition metal catalyst with the metal in a certain oxidation state catalyses the deprotection of a functional group, which in situ undergoes a subsequent transformation catalysed by another complex of the same metal but in a different oxidation state.     

An improved procedure for the palladium-catalyzed oxidative carbonylation of beta-amino alcohols to oxazolidin-2-ones

A highly efficient oxidative cyclocarbonylation of beta-amino alcohols and 2-aminophenol to oxazolidin-2-ones has been achieved by using PdI(2) in conjunction with KI as the catalytic system in DME under relatively mild conditions (100 degrees C and 20 atm of a 4:1 mixture of CO and air).     

Unique phase recovery for nonperiodic objects

It is well known that the loss of phase information at detection means that a diffraction pattern may be consistent with a multitude of physically different structures. This Letter shows that it is possible to perform unique structural determination in the absence of a priori information using x-ray fields with phase curvature. We argue that significant phase curvature is already available using modern x-ray optics and we demonstrate an algorithm that allows the phase to be recovered uniquely and reliably.     

Air-clad optical fibre filament for generating broadband radiation

A simple broadband optical source is demonstrated by using a high numerical aperture air-clad optical fibre to collect broadband emission of blackbody radiation from the fibre during exposure to high intensity electric arcs.     

Investigation of the quantitative properties of the quadrupole orthogonal acceleration time-of-flight mass spectrometer with electrospray ionisation using 3,4-methylenedioxymethamphetamine

This paper describes the investigation of the potential of a quadrupole orthogonal acceleration time-of-flight mass spectrometer (Q-TOF) equipped with an atmospheric pressure ionisation interface for quantitative measurements of small molecules separated by reversed phase liquid chromatography. To this end, the detection limits and linear dynamic range in particular were studied in an LC/MS/MS experiment using 3,4-methylenedioxymethamphetamine standards and 3,4-methylenedioxyethylamphetamine for internal standardisation. In a second phase, the experiment was repeated with real biological extracts (whole blood, serum, and vitreous humour). A calibration for 3,4-methylenedioxymethamphetamine and its metabolite 3,4-methylenedioxyamphetamine was prepared in each of these matrices again using 3,4-methylenedioxyethylamphetamine as internal standard. The resulting quantitative data were compared with those obtained by liquid chromatography with fluorescence detection for the same extracts. The Q-TOF results revealed excellent sensitivity and a linear dynamic range of nearly four decades (2-10 000 pg on-column, r(2) = 0.9998, 1/x weighting). Furthermore, all the calibration curves prepared in biological material were superimposable, LC/MS/MS and LC-fluorescence, and the quantitative results for actual samples compared very favourably. It was concluded that the Q-TOF achieves a linear dynamic range for quantitative LC/MS/MS work exceeding that of fluorescence detection and at much better absolute sensitivity. Copyright 1999 John Wiley & Sons, Ltd.     

Cascade reactions: a new synthesis of 2-benzofuran-2-ylacetamides by sequential Pd(0)-catalyzed deallylation-Pd(II)-catalyzed aminocarbonylative heterocyclization of 1-(2-allyloxyaryl)-2-yn-1-ols

A general and efficient synthesis of 2-benzofuran-2-ylacetamides 5 starting from 1-(2-allyloxyaryl)-2-yn-1-ols 1, amines 4, and CO, in the presence of catalytic amounts of PdI2 in conjunction with PPh3 and KI, has been developed based on the "sequential homobimetallic catalysis" concept, that is, a process in which two different complexes of the same metal, but in two different oxidation states, promote two catalytic cycles in sequence. The first cycle corresponds to a Pd(0)-catalyzed aminodeallylation of 1 with formation of the free phenol 2, which then undergoes Pd(II)-catalyzed aminocarbonylative heterocyclization to give the final product 5.     

Coherence properties of individual femtosecond pulses of an x-ray free-electron laser

Measurements of the spatial and temporal coherence of single, femtosecond x-ray pulses generated by the first hard x-ray free-electron laser, the Linac Coherent Light Source, are presented. Single-shot measurements were performed at 780?eV x-ray photon energy using apertures containing double pinholes in "diffract-and-destroy" mode. We determined a coherence length of 17 μm in the vertical direction, which is approximately the size of the focused Linac Coherent Light Source beam in the same direction. The analysis of the diffraction patterns produced by the pinholes with the largest separation yields an estimate of the temporal coherence time of 0.55?fs. We find that the total degree of transverse coherence is 56% and that the x-ray pulses are adequately described by two transverse coherent modes in each direction. This leads us to the conclusion that 78% of the total power is contained in the dominant mode.     

Rejection of randomly coinciding events in ZnMoO_4 scintillating bolometers

Random coincidence of events (particularly from two neutrino double beta decay) could be one of the main sources of background in the search for neutrinoless double beta decay with cryogenic bolometers due to their poor time resolution. Pulse-shape discrimination by using front edge analysis, mean-time and \(\chi ^2\) methods were applied to discriminate randomly coinciding events in ZnMoO \(_4\) cryogenic scintillating bolometers. These events can be effectively rejected at the level of 99 % by the analysis of the heat signals with rise-time of about 14 ms and signal-to-noise ratio of 900, and at the level of 92 % by the analysis of the light signals with rise-time of about 3 ms and signal-to-noise ratio of 30, under the requirement to detect 95 % of single events. These rejection efficiencies are compatible with extremely low background levels in the region of interest of neutrinoless double beta decay of \(^{100}\) Mo for enriched ZnMoO \(_4\) detectors, of the order of \(10^{-4}\)  counts/(y keV kg). Pulse-shape parameters have been chosen on the basis of the performance of a real massive ZnMoO \(_4\) scintillating bolometer. Importance of the signal-to-noise ratio, correct finding of the signal start and choice of an appropriate sampling frequency are discussed.     

Enriched Zn $$^{100}$$ MoO $$_4$$ scintillating bolometers to search for $$0\nu 2\beta $$ decay of $$^{100}$$ Mo with the LUMINEU experiment

In the present work, we consider a model with a fermionic field that is non-minimally coupled to gravity in the framework of teleparallel gravity. In order to determine the forms of the coupling and potential function of fermionic field for the considered model, we use the Noether symmetry approach. By applying this approach, for the Friedman–Robertson–Walker metric, we obtain the respective potential and coupling functions as a linear and power-law form of the bilinear \(\Psi \) . Furthermore, we search for the exact cosmological solution of the model. It is shown that the fermionic field plays the role of dark energy.     

Tree-Code Based Improvement of Computational Performance of the X-ray-Matter-Interaction Simulation Tool XMDYN

In this work, we report on incorporating for the first time tree-algorithm based solvers into the molecular dynamics code, XMDYN. XMDYN was developed to describe the interaction of ultrafast X-ray pulses with atomic assemblies. It is also a part of the simulation platform, SIMEX, developed for computational single-particle imaging studies at the SPB/SFX instrument of the European XFEL facility. In order to improve the XMDYN performance, we incorporated the existing tree-algorithm based Coulomb solver, PEPC, into the code, and developed a dedicated tree-algorithm based secondary ionization solver, now also included in the XMDYN code. These extensions enable computationally efficient simulations of X-ray irradiated large atomic assemblies, e.g., large protein systems or viruses that are of strong interest for ultrafast X-ray science. The XMDYN-based preparatory simulations can now guide future single-particle-imaging experiments at the free-electron-laser facility, EuXFEL.