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Gas chromatographic investigations of volatile transactinides

English title Gas chromatographic investigations of volatile transactinides
Applicant Eichler Robert
Number 144511
Funding scheme Project funding (Div. I-III)
Research institution Paul Scherrer Institut
Institution of higher education Paul Scherrer Institute - PSI
Main discipline Physical Chemistry
Start/End 01.10.2012 - 30.09.2015
Approved amount 400'715.00
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All Disciplines (3)

Discipline
Physical Chemistry
Inorganic Chemistry
Nuclear Physics

Keywords (6)

transactinides; adsorption; relativistic effects; gas phase chemistry; carbonyl compounds; vacuum chromatography

Lay Summary (German)

Lead
Eine der fundamentalsten Aufgaben der Chemie besteht in der experimentellen chemischen Untersuchung von den schwersten bekannten Elementen (den Transaktinoiden), die es allein möglich macht, den Einfluss der Kernladung auf die Elektronenstruktur der schweren Atome und damit auf ihre chemischen Eigenschaften zu untersuchen.
Lay summary
Mehr als 50 neue Isotope der Transaktinoide wurden in den letzten Jahren in durch Schwerionen induzierten Kernfusionsreaktionen entdeckt. Einig von ihnen haben Halbwertseiten von Einzelsekunden bis zu 32 Stunden. Hinzu kommt die Weiterentwicklung der Technologien der Teilchenbeschleunigung, die für leichtere Transaktinoide bis zum Seaborgium Produktionsraten von bis zu 50 Atomen pro Tag erlauben. Resultate der Untersuchung der Transaktinoide stellen Benchmarkdaten für Theoretische Modelle dar, die relativistische Effekte in den Elektronenstrukturen alle Elemente quantifizieren können. In zwei Doktorarbeiten untersuchen wir:
A.) Die Gasphasenchemie von Verbindungen tiefer Oxidationsstufen von Transaktinoiden im Übergangsmetallbereich des Periodensystems anhand ihrer flüchtigen Carbonylverbindungen. Wir erarbeiten eine Methode, mit welcher die thermische Stabilität von Carbonylmolekülen der Gruppe 6 untersucht werden kann, welche Rückschüsse auf relativistische Effekte innerhalb des Moleküls erlaubt.
B.) Die Möglichkeiten der Weiterentwicklung ultraschneller Gaschromatographie im Vakuum soll zukünftig die führende Rolle unserer Gruppe bei der Untersuchung der superschweren Elemente 112-116 sichern.
Direct link to Lay Summary Last update: 12.08.2014

Responsible applicant and co-applicants

Employees

Publications

Publication
Decomposition studies of group 6 hexacarbonyl complexes. Part 1: Production and decomposition of Mo(CO)6 and W(CO)6
Usoltsev I., Eichler R., Wang Y., Even J., Yakushev A., Haba H., Asai M., Brand H., Di Nitto A., Düllmann Ch.E., Fangli F., Hartmann W., Huang M., Jäger E., Kaji D., Kanaya J., Kaneya Y., Khuyagbaatar J., Kindler B., Kratz J.V., Krier J., Kudou Y., Kurz N., Lommel B., et al. (2016), Decomposition studies of group 6 hexacarbonyl complexes. Part 1: Production and decomposition of Mo(CO)6 and W(CO)6, in Radiochimica Acta, 104(3), 141.
Decomposition studies of group 6 hexacarbonyl complexes. Part 2: Modelling of the decomposition process
Usoltsev Ilya, Eichler Robert, Türler Andreas (2016), Decomposition studies of group 6 hexacarbonyl complexes. Part 2: Modelling of the decomposition process, in Radiochimica Acta, 104(8), 531.
Chemical studies of elements with Z⩾104 in gas phase
Türler Andreas, Eichler Robert, Yakushev Alexander (2015), Chemical studies of elements with Z⩾104 in gas phase, in Nuclear Physics A, 944, 640-689.
In situ synthesis of volatile carbonyl complexes with short-lived nuclides
Even Julia, Ackermann Dieter, Asai Masato, Block Michael, Brand Holger, Di Nitto Antonio, Duellmann Christoph E., Eichler Robert, Fan Fangli, Haba Hiromitsu, Hartmann Willi, Huebner Annett, Hessberger Fritz P., Huang Minqhiu, Jaeger Egon, Kaji Daiya, Kanaya Jumpei, Kaneya Yusuke, Khuyagbaatar Jadambaa, Kindler Birgit, Kratz Jens V., Krier Joerg, Kudou Yuki, Kurz Nikolaus, Laatiaoui Mustapha (2015), In situ synthesis of volatile carbonyl complexes with short-lived nuclides, in JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY, 303(3), 2457-2466.
Vapor deposition coating of fused silica tubes with amorphous selenium
Chiera N.M., Eichler R., Vögele A., Türler A. (2015), Vapor deposition coating of fused silica tubes with amorphous selenium, in Thin Solid Films, 592, 8-13.
First principles based modeling of the adsorption of atoms of element 120 on a gold surface
Demidov Yuriy, Zaitsevskii Andréi, Zaitsevskii Andréi, Eichler Robert, Eichler Robert (2014), First principles based modeling of the adsorption of atoms of element 120 on a gold surface, in Physical Chemistry Chemical Physics, 16(6), 2268-2270.
In-situ formation, thermal decomposition, and adsorption studies of transition metal carbonyl complexes with short-lived radioisotopes
Even Julia, Yakushev Alexander, Duellmann Christoph Emanuel, Dvorak Jan, Eichler Robert, Gothe Oliver, Hartmann Willy, Hild Daniel, Jaeger Egon, Khuyagbaatar Jadambaa, Kindler Birgit, Kratz Jens Volker, Krier Joerg, Lommel Bettina, Niewisch Lorenz, Nitsche Heino, Pysmenetska Inna, Schaedel Matthias, Schausten Brigitta, Tuerler Andreas, Wiehl Norbert, Wittwer David (2014), In-situ formation, thermal decomposition, and adsorption studies of transition metal carbonyl complexes with short-lived radioisotopes, in RADIOCHIMICA ACTA, 102(12), 1093-1110.
Pioneering experiments on the chemical properties of element 113
Dmitriev Sergey N., Aksenov Nikolay V., Albin Yuriy V., Bozhikov Gospodin A., Chelnokov Maxim L., Chepygin Viktor I., Eichler Robert, Isaev Andrei V., Katrasev Denis E., Lebedev Vyacheslav Ya, Malyshev Oleg N., Petrushkin Oleg V., Porobanuk Lidia S., Ryabinin Mikhail A., Sabel'nikov Alexey V., Sokol Evgeny A., Svirikhin Alexander V., Starodub Gennadii Ya, Usoltsev Ilya, Vostokin Grigory K., Yeremin Alexander V. (2014), Pioneering experiments on the chemical properties of element 113, in MENDELEEV COMMUNICATIONS, 24(5), 253-256.
Superheavy element chemistry
Eichler Robert (2014), Superheavy element chemistry, in W. Greiner (ed.), Springer, Heidelberg, 33-43.
Synthesis and detection of a seaborgium carbonyl complex
Even J., Yakushev A., Duellmann Ch E., Haba H., Asai M., Sato T. K., Brand H., Di Nitto A., Eichler R., Fan F. L., Hartmann W., Huang M., Jaeger E., Kaji D., Kanaya J., Kaneya Y., Khuyagbaatar J., Kindler B., Kratz J. V., Krier J., Kudou Y., Kurz N., Lommel B., Miyashita S., Morimoto K. (2014), Synthesis and detection of a seaborgium carbonyl complex, in SCIENCE, 345(6203), 1491-1493.
Adsorption interaction of carrier-free thallium species with gold and quartz surfaces
Serov A., Serov A., Eichler R., Eichler R., Eichler R., Dressler R., Piguet D., Türler A., Türler A., Vögele A., Wittwer D., Wittwer D., Gäggeler H. W., Gäggeler H. W. (2013), Adsorption interaction of carrier-free thallium species with gold and quartz surfaces, in Radiochimica Acta, 101(7), 421-425.
Advances in the Production and Chemistry of the Heaviest Elements
Tuerler Andreas, Pershina Valeria (2013), Advances in the Production and Chemistry of the Heaviest Elements, in CHEMICAL REVIEWS, 113(2), 1237-1312.
Experimental techniques
Türler Andreas, Türler Andreas, Gregorich Kenneth E. (2013), Experimental techniques, in M. Schädel & D. Shaughnessy (ed.), Springer, Berlin Heidelberg, 261-308.
First foot prints of chemistry on the shore of the Island of superheavy elements
Eichler R., Eichler R. (2013), First foot prints of chemistry on the shore of the Island of superheavy elements, in Journal of Physics: Conference Series, 420(1), 12003.
Gas-phase chemistry of superheavy elements
Gäggeler Heinz W., Gäggeler Heinz W., Türler Andreas, Türler Andreas (2013), Gas-phase chemistry of superheavy elements, in M. Schädel & D. Shaughnessy (ed.), Springer, Berlin Heidelberg, 415-483.
Prediction of the thermal release of transactinide elements (112≤Z≤116) from metals
Wittwer D., Wittwer D., Dressler R., Eichler R., Eichler R., Gäggeler H. W., Gäggeler H. W., Türler A., Türler A. (2013), Prediction of the thermal release of transactinide elements (112≤Z≤116) from metals, in Radiochimica Acta, 101(4), 211-219.
Preparation and high intensity heavy ion irradiation tests of intermetallic Am-243/Pd targets
Usoltsev I., Eichler R., Vostokin G. K., Sabel'nikov A. V., Aksenov N. V., Albin Y. V., Bozhikov G. A., Chepigin V. I., Dmitriev S. N., Lebedev V. Ya., Malyshev O. N., Petrushkin O. V., Piguet D., Starodub G. Ya, Svirikhin A. I., Tuerler A., Yeremin A. V. (2013), Preparation and high intensity heavy ion irradiation tests of intermetallic Am-243/Pd targets, in NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATO, 318, 297-305.
Thermal release rate studies of nuclear reaction products from polycrystalline metal matrices
Wittwer D., Wittwer D., Dressler R., Eichler R., Eichler R., Gäggeler H. W., Gäggeler H. W., Piguet D., Türler A., Türler A. (2013), Thermal release rate studies of nuclear reaction products from polycrystalline metal matrices, in Nuclear Instruments and Methods in Physics Research, Section B: Beam Interactions with Materials and, 297, 86-93.
Thermochemical data from gas-phase adsorption and methods of their estimation
Eichler Robert, Eichler Bernd (2013), Thermochemical data from gas-phase adsorption and methods of their estimation, in M. Schädel & D. Shaughnessy (ed.), Springer, Berlin Heidelberg, 375-413.
Preparation of Pd-based intermetallic targets for high intensity irradiations
Usoltsev I., Eichler R., Dressler R., Piguet D., Wittwer D., Tuerler A., Bruetsch R., Olsen E. A., Omtvedt J. P., Semchenkov A. (2012), Preparation of Pd-based intermetallic targets for high intensity irradiations, in NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION A-ACCELERATORS SPECTROMETERS DETECTORS AND, 691, 5-9.
Rapid Synthesis of Radioactive Transition-Metal Carbonyl Complexes at Ambient Conditions
Even Julia, Yakushev Alexander, Duellmann Christoph E., Dvorak Jan, Eichler Robert, Gothe Oliver, Hild Daniel, Jaeger Egon, Khuyagbaatar Jadambaa, Kratz Jens V., Krier Joerg, Niewisch Lorenz, Nitsche Heino, Pysmenetska Inna, Schaedel Matthias, Schausten Brigitta, Tuerler Andreas, Wiehl Norbert, Wittwer David (2012), Rapid Synthesis of Radioactive Transition-Metal Carbonyl Complexes at Ambient Conditions, in INORGANIC CHEMISTRY, 51(12), 6431-6433.
Study of the average charge states of 188Pb and 252,254No ions at the gas-filled separator TASCA
Khuyagbaatar J., Khuyagbaatar J., Ackermann D., Andersson L. L., Andersson L. L., Ballof J., Brüchle W., Düllmann Ch E., Düllmann Ch E., Düllmann Ch E., Dvorak J., Dvorak J., Eberhardt K., Even J., Gorshkov A., Graeger R., Heßberger F. P., Heßberger F. P., Hild D., Hoischen R., Hoischen R., Jäger E., Kindler B., Kratz J. V., Lahiri S. (2012), Study of the average charge states of 188Pb and 252,254No ions at the gas-filled separator TASCA, in Nuclear Instruments and Methods in Physics Research, Section A: Accelerators, Spectrometers, Detecto, 689, 40-46.

Collaboration

Group / person Country
Types of collaboration
SAFE-OCL /Oslo University Norway (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
Heavy Elements Group / LBNL Berkeley United States of America (North America)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Superheavy Element Laboratory/RIKEN-Nishina Japan (Asia)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
Japan Atomic Energy Agency (ASRC) Japan (Asia)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
FLNR Dubna Russia (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel
Heavy Elements / Helmholtz Institute Mainz Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Nuclear Chemistry Division/ GSI Darmstadt Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
Institut für Kernchemie/University Mainz Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
5th International Conference on the Chemistry and Physics of the Transactinide Elements TAN Talk given at a conference Can NO replace CO for formation of volatile compounds with d-elements? 25.05.2015 Urabandai, Japan Eichler Robert;
5th International Conference on the Chemistry and Physics of the Transactinide Elements TAN Talk given at a conference On-line Isothermal Vacuum Chromatography (IVAC) of Tl on Quartz 25.05.2015 Urabandai, Japan Steinegger Patrick Julian Rolf;
5th International Conference on the Chemistry and Physics of the Transactinide Elements TAN Talk given at a conference Chemistry Experiments for Transactinide Elements 25.05.2015 Urabandai, Japan Türler Andreas;
5th International Conference on the Chemistry and Physics of the Transactinide Elements TAN Talk given at a conference Probing the thermal stability of group VI metal hexacarbonyl complexes 25.05.2015 Urabandai, Japan Eichler Robert;
17th Radiochemical Conference Talk given at a conference Decomposition studies of W and Mo carbonyl complexes and their implications for future experiments with Sg(CO)6 11.05.2014 Marianske Lazne, Czech Republic Usoltsev Ilya;
5th Asia-Pacific Symposium on Radiochemistry APSORC’13 Talk given at a conference Diamond Detectors for Isothermal Vacuum Chromatography 22.09.2013 Kanazawa, Japan Steinegger Patrick Julian Rolf;
5th Asia-Pacific Symposium on Radiochemistry APSORC’13 Talk given at a conference Intermetallic Actinide Compounds for SHE Production Targets 22.09.2013 Kanazawa, Japan Eichler Robert;
5th Asia-Pacific Symposium on Radiochemistry APSORC’13 Talk given at a conference Advances in the production and chemistry of the heaviest elements 22.09.2013 Kanazawa, Japan Türler Andreas;
5th Asia-Pacific Symposium on Radiochemistry APSORC’13 Talk given at a conference New insights into the formation and stability of Molybdenum carbonyl compounds 22.09.2013 Kanazawa, Japan Usoltsev Ilya;
GDCh-Wissenschaftsforum Chemie 2013 Talk given at a conference Synthese und charakterisierung superschwerer Elemente 01.09.2013 Darmstadt, Germany Türler Andreas;
Symposium on Nuclear Physics: Presence and Future Talk given at a conference Superheavy Element Chemistry – Achievements and Prospective 29.05.2013 Boppard, Germany Eichler Robert;


Communication with the public

Communication Title Media Place Year
Media relations: print media, online media Experimente am Ende des Periodensystems NZZ German-speaking Switzerland 2013
Media relations: print media, online media Neuen Elementen auf der Spur Blick am Abend German-speaking Switzerland 2013

Awards

Title Year
1st Year Graduate Symposium Award; Department of Chemistry and Biochemistry, University of Bern 2013

Associated projects

Number Title Start Funding scheme
162769 Gas chromatographic investigations of volatile transactinides 01.02.2016 Project funding (Div. I-III)
126639 Gas chromatographic investigations of volatile transactinides 01.10.2009 Project funding (Div. I-III)

Abstract

A world-wide boost in the transactinide research can be observed. New accelerator facilities and separator setups are planned or are already being built at the large accelerator centers in Germany, Russia, and Japan. The exciting results from the physics investigation of transactinides revealed a new member of the periodic table, element 117. Further experiments aimed at the discovery of the elements 119 and 120 are ongoing at GSI Darmstadt, Germany. More than 50 new isotopes of transactinides have been discovered in the recent years. Some of them have half-lives from single seconds up to 32 hours. Moreover, the developments in accelerator techniques and target technology allow for unprecedented production rates for lighter transactinides (e.g. Sg) of 50 atoms per day. Physical preseparation assists the chemical setups to further suppress background and to unambiguously identify the single atoms of transactinides. The fundamental chemical investigation of transactinides allows assessing the atomic structure of the elements at the very edge of the periodic table influenced be the increasingly high nuclear charge inducing relativistic effects. Hence, the results of these investigations represent benchmark data for models used in theoretical chemistry. Furthermore, the investigation of the lighter homologues of the transactinides in the corresponding groups of the periodic table at single atomic concentrations yield fascinating new physico-chemical data for elements, which previously appeared to be well known.We propose here two PHD projects, which are connected to the most exciting research tasks recently emerging from the field of transactinide chemistry:A.) The gas phase investigation of low oxidation state compounds of transition metal transactinides in the form of carbonyls. The relativistic effects are expected to be stronger expressed in the chemical properties of so far out of reach low oxidation states of the lighter transactinides Rf-Mt. Therefore, we propose here to investigate the thermal stability of carbonyl complex compounds recently observed in on-line chemical investigations with short-lived isotopes of the lighter homologues of these elements.B.) The further development of the ultra fast technique of high temperature vacuum chromatography suitable for the first chemical investigation of the superheavy elements 113-116.
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