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Gas chromatographic investigations of volatile transactinides

English title Gas chromatographic investigations of volatile transactinides
Applicant Eichler Robert
Number 162769
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 01.02.2016 - 31.01.2020
Approved amount 529'332.00
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All Disciplines (3)

Discipline
Physical Chemistry
Inorganic Chemistry
Nuclear Physics

Keywords (7)

carbonyl complex compounds; transactinides; adsorption gas phase chromatography; vacuum chromatography; relativistic effects; single atom chemistry; on-line separation

Lay Summary (German)

Lead
Transaktinoidenchemie, bekannt auch als Chemie Superschwerer Elemente, beprobt experimentell eines der fundamentalsten Ordnungsschemata der chemischen Elemente - das Periodensystem - an seiner schwersten Grenze. Die Resultate dieser Forschung liefern Benchmarkdaten für moderne theoretische Berechnungsmodelle, die auf unserem heutigen Verständnis des Einflusses der hohen Kernladung auf die Elektronenstruktur der Atome basieren..
Lay summary
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. Erst kürzlich wurde die Entdeckung von vier neuen Elementen von der IUPAC akzeptiert. Mehr als 50 neue Isotope der Transaktinoide  mit Halbwertseiten von Millisekunden bis zu einigen Stunden in den letzten Jahren in durch Schwerionen induzierten Kernfusionsreaktionen entdeckt. 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 des Periodensystems quantifizieren können. In zwei Doktorarbeiten untersuchen wir:
A.) Die Gasphasenchemie von Verbindungen tiefer Oxidationsstufen von Transaktinoiden im Übergangsmetallbereich des Periodensystems Sg-Mt anhand ihrer flüchtigen Carbonylverbindungen. Wir erarbeiten eine Methode, mit welcher die thermische Stabilität von Carbonylmolekülen untersucht werden kann, welche Rückschüsse auf relativistische Effekte innerhalb des Moleküls erlaubt.
B.) Die Möglichkeiten der Weiterentwicklung ultraschneller Gaschromatographie im Vakuum soll zukünftig die Untersuchung sehr kurzlebiger Isotope der superschweren Elemente 113-118 in weit unter einer Sekunde ermöglichen.
Direct link to Lay Summary Last update: 20.01.2016

Lay Summary (English)

Lead
Transactinide chemistry, often referred to as superheavy element chemistry, challenges experimentally one of the most fundamental ordering schemes of chemical elements - the periodic table. The results of this research benchmark the current theoretical understanding of the influence of high nuclear charges on the atomic structure of elements.
Lay summary

The fundamental chemical investigation of transactinides allows assessing the atomic structure of the heaviest elements at the very border of the periodic table influenced by the increasingly high nuclear charge inducing strong relativistic effects. Recently, the discovery of four new elements has been accepted by IUPAC. More than 50 new isotopes of superheavy elements have been discovered in the recent years with half-lives ranging from milliseconds up to several hours.  Moreover, the developments in accelerator techniques and target technology allow nowadays for unprecedented production rates for lighter transactinides (e.g. Sg) of 50 atoms per day. The results of these challenging fast experimental investigations at the one-atom-at-a-time level represent benchmark data for models used in theoretical chemistry describing chemical properties of the elements in the periodic table. Within two PHD projects we investigate:

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 technical possibilities for the development of a new ultra fast technique of high temperature vacuum chromatography suitable on the longer-term for the first-time chemical investigation of the superheavy elements with Z=115-118, having half-lives well below one second.

Direct link to Lay Summary Last update: 20.01.2016

Responsible applicant and co-applicants

Employees

Publications

Publication
The periodic table – an experimenter’s guide to transactinide chemistry
Eichler Robert (2019), The periodic table – an experimenter’s guide to transactinide chemistry, in Radiochimica Acta, 107(9-11), 865-877.
Reactions of fission products from a 252Cf source with NO and mixtures of NO and CO in an inert gas
Gäggeler Heinz W., Usoltsev Ilya, Eichler Robert (2019), Reactions of fission products from a 252Cf source with NO and mixtures of NO and CO in an inert gas, in Radiochimica Acta, 107(7), 555-560.
The Periodic Table of Elements: Superheavy in Chemistry
Eichler Robert (2019), The Periodic Table of Elements: Superheavy in Chemistry, in Nuclear Physics News, 29(1), 11-15.
The study of rhenium pentacarbonyl complexes using single-atom chemistry in the gas phase
Wang Yang, Cao Shiwei, Zhang Jicai, Fan Fangli, Yang Jie, Haba Hiromitsu, Komori Yukiko, Yokokita Takuya, Morimoto Kouji, Kaji Daiya, Wittwer Yves, Eichler Robert, Türler Andreas, Qin Zhi (2019), The study of rhenium pentacarbonyl complexes using single-atom chemistry in the gas phase, in Physical Chemistry Chemical Physics, 21(13), 7147-7154.
Superheavy Element Chemistry—New Experimental Results Challenge Theoretical Understanding In: New Horizons in Fundamental Physics
Eichler R. (2017), Superheavy Element Chemistry—New Experimental Results Challenge Theoretical Understanding In: New Horizons in Fundamental Physics, Springer International Publishing, Cham.
Diamond detectors for high-temperature transactinide chemistry experiments
Steinegger Patrick, Dressler Rugard, Eichler Robert, Piguet Dave, Streuli Silvan, Türler Andreas (2017), Diamond detectors for high-temperature transactinide chemistry experiments, in Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detector, 850, 61-67.
Complex chemistry with complex compounds
Eichler Robert, Asai M., Brand H., Chiera N.M., Di Nitto A., Dressler R., Düllmann Ch.E., Even J., Fangli F., Goetz M., Haba H., Hartmann W., Jäger E., Kaji D., Kanaya J., Kaneya Y., Khuyagbaatar J., Kindler B., Komori Y., Kraus B., Kratz J.V., Krier J., Kudou Y., Kurz N., et al. (2016), Complex chemistry with complex compounds, in EPJ Web of Conferences, 131, 07005-07005.
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), 141-151.
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), 531-537.

Collaboration

Group / person Country
Types of collaboration
Nuclear Chemistry Division/ GSI Darmstadt Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
Superheavy Element Laboratory/RIKEN-Nishina 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
Institut für Kernchemie/University Mainz Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Exchange of personnel
Heavy Elements / Helmholtz Institute Mainz Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Exchange of personnel
Heavy Elements group / ASRC Japan Atomic Energy Agency Japan (Asia)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
4th International Symposium Super Heavy Elements (SHE2019) Talk given at a conference Current and Future Chemistry Experiments with Transactinides 01.12.2019 Hakone, Japan Eichler Robert;
18-th TASCA Workschop Talk given at a conference Optimizing the in-situ production yield of transition metal carbonyls 25.09.2019 Darmstadt, Germany Wittwer Yves Jean-Jacques;
XXI Mendeleev Congress General and Applied Chemistry Talk given at a conference The Periodic Table a Driver for Transactinide Chemistry 09.09.2019 St.Petersburg, Russia Eichler Robert;
6-th International Conference on the Chemistry and Physics of the Transactinide Elements (TAN19) Poster Vacuum Chromatography on the Long Hard Road to the Accelerator 25.08.2019 Wilhelmshaven, Germany Kraus Benjamin;
6-th International Conference on the Chemistry and Physics of the Transactinide Elements (TAN19) Talk given at a conference Optimization of Transactinide Carbonyl Complex Formation and Transport using Fission Products from Cf-252 25.08.2019 Wilhelmshaven, Germany Wittwer Yves Jean-Jacques;
Russian Academy of Science Symposium on Heaviest Elements Individual talk Status and Prospects of Gas Phase Chemistry with Transactinides 30.05.2019 Dubna, Russia Eichler Robert;
International symposium “The present and the future of the Periodic Table of Chemical Elements” Individual talk Prospects of Gas Phase Chemistry with Short-lived Transactinides “microsecond chemistry?” 30.05.2019 Dubna, Russia Eichler Robert;
7th ADAMAS Workshop Talk given at a conference High-Temperature α-Spectroscopy with Diamond-based Detectors 13.12.2018 Vienna, Austria Kraus Benjamin;
18th Radiochemical Conference Talk given at a conference Diamond-based detectors for future chemistry experiments with superheavy elements 13.05.2018 Mariánské Lászně, Czech Republic Kraus Benjamin;
18th Radiochemical Conference Poster On the formation and stability of metal carbonyl complexes from superheavy elements and their homologues 13.05.2018 Mariánské Lászně, Czech Republic Wittwer Yves Jean-Jacques;
Working Meeting on the Prospects of Research on the Chemistry of Superheavy Elements at the new SHE factory Individual talk Prospects for Superheavy Element Chemistry 06.12.2017 Dubna, Russia Eichler Robert;
9-th Workshop on the Chemistry of the Heaviest Elements Talk given at a conference Getting insights into the metal-carbonyl complex formation 08.10.2017 Ascona, Switzerland Wittwer Yves Jean-Jacques;
9-th International Workshop on the Chemistry of the Heaviest Elements (CHE9) Talk given at a conference Isothermal vacuum chromatography of Pb on quartz as model to investigate superheavy elements 01.10.2017 Ascona, Switzerland Kraus Benjamin;
GDCh – Wissenschaftsforum Chemie 2017 Poster Getting insights into the metal-carbonyl complex formation 10.09.2017 Berlin, Germany Wittwer Yves Jean-Jacques;
GDCh – Wissenschaftsforum Chemie 2017 Poster Isothermal vacuum chromatography of Pb on quartz as model to investigate superheavy elements 10.09.2017 Berlin, Germany Kraus Benjamin;
3rd International Symposium on Super-Heavy Elements Talk given at a conference Challenges in the studies of super-heavy nuclei and atoms 10.09.2017 Kazimierz-Dolny, Poland Eichler Robert;
Colloquium: Element Inauguration Moscovium, Tennessine, Oganesson Individual talk Superheavy Element Chemistry 03.03.2017 Dubna, Russia Eichler Robert;
9th International Conference on Nuclear and Radiochemistry NRC9 Talk given at a conference Experimentally assessing the metal-carbon bond stability in Sg(CO)6 29.08.2016 Helsinki, Finland Eichler Robert;
Nobel Symposium NS160 - Chemistry and Physics of Heavy and Superheavy Element Talk given at a conference Complex Chemistry with Metal complexes 29.05.2016 Scania, Sweden Eichler Robert;
Nobel Symposium NS160 - Chemistry and Physics of Heavy and Superheavy Element Talk given at a conference Advances in Chemical Investigations of Heaviest Elements 29.05.2016 Scania, Sweden Türler Andreas;


Self-organised

Title Date Place
9-th International Workshop on the Chemistry of the Heaviest Elements (CHE9) 08.10.2017 Ascona, Switzerland

Awards

Title Year
1st place students poster presentation @ 18th Radiochemical Conference, Mariánské Lázně, Czech Republic 2018

Associated projects

Number Title Start Funding scheme
196981 Gas chromatographic investigations of volatile transactinides 01.01.2021 Project funding (Div. I-III)
144511 Gas chromatographic investigations of volatile transactinides 01.10.2012 Project funding (Div. I-III)

Abstract

The chemical investigation of transactinide elements queries one of the most fundamental chemical questions regarding the validity of the rules of periodicity established by the periodic table of elements at its heaviest edges. The achieved experimental data represent benchmark values for the most modern calculation models based on fully-relativistic density functional theory.Generally, the investigation of transactinide elements approaches a new era. Within the next 2-4 years the upcoming availability of new accelerator facilities in Russia, France, Germany, and Japan combined with highly efficient physical separator systems will allow transactinide experiments on an unprecedented sensitivity level. This prospective advocates a strong research commitment in the exciting field of transactinide research. The current project focuses therefore, on the development of chemical methods suitable to investigate the properties of the heaviest elements which will remain available only in single atomic amounts at a time. Therefore, we pursue further our successful strategy to combine the development of fast classical gas-jet based gas chromatography systems (Project A) with the challenging development of an ultra-fast vacuum chromatography (Project B). Both developments have advantages and disadvantages depending on the investigated chemical system and on the nuclear decay properties of the investigated SHE nuclides. Thus, both developments are important to maintain a leading position in this research area:Project A.) The gas phase investigation of low oxidation state compounds of transition metal transactinides in the form of carbonyls based on classical gas chromatography schemes. After the successful chemical identification of Sg(CO)6 and the development of a thermal decomposition setup enabling to assess for the first time the chemical bond strength in a transactinide molecule, we propose here to investigate the thermal stability od Sg(CO)6 and to develop further the even more challenging equivalent investiga-tion of carbonyl complex compounds of the transition metals of group 7-9 of the periodic table. This project in-tends to culminate in two major highlights: The first assessment of a chemical bond strength in a transactinide molecule at its lowest zero-oxidation state, i.e. with all electrons present, for element seaborgium (element 106), and second, as a longer term goal, the first ever chemical investigation of element meitnerium (element 109).Project B.) The development of the ultra-fast high temperature vacuum chromatography technique suitable for the first chemical investigation of the superheavy elements 113-118.After a highly sophisticated technological development regarding the thermal release of single atoms form high melting solid materials and the development of high temperature diamond detectors achieved within in the previous funding periods this project part culminated recently in the successful proof-of-principle isothermal vacuum chromatography experiment (IVAC) with short-lived alpha decaying isotopes of element Tl, the lighter homologue of element 113. In the course of the current project we intend to enter now the speed and efficiency optimization phase for IVAC, which requires largely on-line experimental work optimizing the size and geometry of the catcher-release part of the setup, of the chromatography oven, and improving the particle detection efficiency using the diamond detectors.
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