Experimental investigations of transactinoide elements provide benchmark results for chemical theory and probe the predictive power of trends in the periodic table. So far, in gas-phase chemical reactions, simple inorganic compounds with the transactinoide in its highest oxidation state have been synthesized. Single-atom production rates, short half-lives, and harsh experimental conditions limited the number of experimentally accessible compounds. We applied a gas-phase carbonylation technique previously tested on short-lived molybdenum (Mo) and tungsten (W) isotopes to the preparation of a carbonyl complex of seaborgium, the 106th element. The volatile seaborgium complex showed the same volatility and reactivity with a silicon dioxide surface as those of the hexacarbonyl complexes of the lighter homologs Mo and W. Comparison of the product's adsorption enthalpy with theoretical predictions and data for the lighter congeners supported a Sg(CO)6 formulation.
Chemical studies of superheavy elements require fast and efficient techniques, due to short half-lives and low production rates of the investigated nuclides. Here, we advocate for using a tubular flow reactor for assessing the thermal stability of the Sg carbonyl complexSg(CO) 6 . The experimental setup was tested with Mo and W carbonyl complexes, as their properties are established and supported by theoretical predictions. The suggested approach proved to be effective in discriminating between the thermal stabilities of Mo(CO) 6 and W(CO) 6 . Therefore, an experimental verification of the predicted Sg−CO bond dissociation energy seems to be feasible by apply- Tc carbonyl complex, we estimated the lower reaction time limit for the metal carbonyl synthesis in the gas phase to be more than 100 ms. We examined further the influence of the wall material of the recoil chamber, the carrier gas composition, the gas flow rate, and the pressure on the production yield of 104 Mo(CO) 6 , so that the future stability tests with Sg(CO) 6 can be optimized accordingly.
The detection of VUV scintillation light, e.g. in (liquid) argon detectors, commonly includes a reflector with a fluorescent coating, converting UV photons to visible light. The light yield of these detectors depends directly on the conversion efficiency. Several coating/reflector combinations were produced using VM2000, a specular reflecting multi layer polymer, and Tetratex R a diffuse reflecting PTFE fabric, as reflector foils. The light yield of these coatings was optimised and has been measured in a dedicated liquid argon setup built at the University of Zurich. It employs a small, 1.3 kg LAr cell viewed by a 3-inch, low radioactivity PMT of type R11065-10 from Hamamatsu. The cryogenic stability of these coatings was additionally studied. The optimum reflector/coating combination was found to be Tetratex R dip coated with Tetraphenyl-butadiene with a thickness of 0.9 mg/cm 2 resulting in a 3.6 times higher light yield compared to uncoated VM2000. Its performance was stable in long term measurements, ran up to 100 days, in liquid argon. This coated reflector was further investigated concerning radioactive impurities found to be suitable for current and upcoming low-background experiments. Therefore it is used for the liquid argon veto in Phase II of the GERDA neutrinoless double beta decay experiment.
Abstract:The decomposition behavior of group 6 metal hexacarbonyl complexes (M(CO) 6 ) in a tubular flow reactor is simulated. A microscopic Monte-Carlo based model is presented for assessing the first bond dissociation enthalpy of M(CO) 6 complexes. The suggested approach superimposes a microscopic model of gas adsorption chromatography with a first-order heterogeneous decomposition model. The experimental data on the decomposition of Mo(CO) 6 and W(CO) 6 are successfully simulated by introducing available thermodynamic data. Thermodynamic data predicted by relativistic density functional theory is used in our model to deduce the most probable experimental behavior of the corresponding Sg carbonyl complex. Thus, the design of a chemical experiment with Sg(CO) 6 is suggested, which is sensitive to benchmark our theoretical understanding of the bond stability in carbonyl compounds of the heaviest elements.
Rapid in situ formation of metal carbonyl complexes with short-lived nuclides has been demonstrated to be feasible with recoiling ions formed in nuclear fusion and fission reactions. These carbonyl complexes are highly volatile and can be transported rapidly in a gas-stream to counting or chemistry devices. This method was already successfully applied in the chemical investigation of the superheavy element seaborgium (Z = 106) and appears promising for various fields of nuclear research. In this article, we give an overview on the current status of metal carbonyl complex studies with short-lived d-element isotopes.
Abstract. In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the investigation of fragile single molecular species by gas-phase chromatography. The latest success with the heaviest group 6 transactinide seaborgium is highlighted. The formation of a very volatile hexacarbonyl compound Sg(CO) 6 was observed similarly to its lighter homologues molybdenum and tungsten. The interactions of these gaseous carbonyl complex compounds with quartz surfaces were investigated by thermochromatography. Second-generation experiments are under way to investigate the intramolecular bond between the central metal atom of the complexes and the ligands addressing the influence of relativistic effects in the heaviest compounds. Our contribution comprises some aspects of the ongoing challenging experiments as well as an outlook towards other interesting compounds related to volatile complex compounds in the gas phase.
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