To search for the lowest energy nuclear isomeric transition in 229 Th in solid samples, a novel adsorption technique which prepares 229 Th atoms on a surface of CaF 2 is developed. Adsorbed 229 Th is exposed to highly intensive undulator radiation in the wavelength range between 130 and 320 nm, which includes the indirectly measured nuclear resonance wavelength 160(10) nm. After the excitation, fluorescence from the sample is detected with a VUV sensitive photomultiplier tube. No clear signal relating to the nuclear transition is observed and possible reasons are discussed.
Recently, it has been shown that experimental data from angle-resolved photoemission spectroscopy on oriented molecular films can be utilized to retrieve real-space images of molecular orbitals in two dimensions. Here, we extend this orbital tomography technique by performing photoemission initial state scans as a function of photon energy on the example of the brickwall monolayer of 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA) on Ag(110). The overall dependence of the photocurrent on the photon energy can be well accounted for by assuming a plane wave for the final state. However, the experimental data, both for the highest occupied and the lowest unoccupied molecular orbital of PTCDA, exhibits an additional modulation attributed to final state scattering effects. Nevertheless, as these effects beyond a plane wave final state are comparably small, we are able, with extrapolations beyond the attainable photon energy range, to reconstruct three-dimensional images for both orbitals in agreement with calculations for the adsorbed molecule.
We aim to perform direct optical spectroscopy of the 229 Th nuclear isomer to measure its energy and lifetime, and to demonstrate optical coupling to the nucleus. To this end, we develop 229 Thdoped CaF2 crystals, which are transparent at the anticipated isomer wavelength. Such crystals are illuminated by tunable VUV undulator radiation for direct excitation of the isomer. We scan a ±5 σ region around the assumed isomer energy of 7.8(5) eV and vary the excitation time in sequential scans between 30 and 600 seconds. Suffering from an unforeseen strong photoluminescence of the crystal, the experiment is sensitive only to radiative isomer lifetimes between 0.2 and 1.1 seconds. For this parameter range, and assuming radiative decay as the dominant de-excitation channel, we can exclude an isomer with energy between 7.5 and 10 eV at the 95% confidence level.
The determination of reaction pathways and the identification of reaction intermediates are key issues in chemistry. Surface reactions are particularly challenging, since many methods of analytical chemistry are inapplicable at surfaces. Recently, atomic force microscopy has been employed to identify surface reaction intermediates. While providing an excellent insight into the molecular backbone structure, atomic force microscopy is less conclusive about the molecular periphery, where adsorbates tend to react with the substrate. Here we show that photoemission tomography is extremely sensitive to the character of the frontier orbitals. Specifically, hydrogen abstraction at the molecular periphery is easily detected, and the precise nature of the reaction intermediates can be determined. This is illustrated with the thermally induced reaction of dibromo-bianthracene to graphene which is shown to proceed via a fully hydrogenated bisanthene intermediate. We anticipate that photoemission tomography will become a powerful companion to other techniques in the study of surface reaction pathways.
A novel X-ray gas monitor (XGM) has been developed which allows the measurement of absolute photon pulse energy and photon beam position at all existing and upcoming free-electron lasers (FELs) over a broad spectral range covering vacuum ultraviolet (VUV), extreme ultraviolet (EUV) and soft and hard X-rays. The XGM covers a wide dynamic range from spontaneous undulator radiation to FEL radiation and provides a temporal resolution of better than 200 ns. The XGM consists of two X-ray gas-monitor detectors (XGMDs) and two huge-aperture open electron multipliers (HAMPs). The HAMP enhances the detection efficiency of the XGM for low-intensity radiation down to 105 photons per pulse and for FEL radiation in the hard X-ray spectral range, while the XGMD operates in higher-intensity regimes. The relative standard uncertainty for measurements of the absolute photon pulse energy is well below 10%, and down to 1% for measurements of relative pulse-to-pulse intensity on pulses with more than 1010 photons per pulse. The accuracy of beam-position monitoring in the vertical and horizontal directions is of the order of 10 µm.
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