Vacuum Chromatography of Tl on SiO2 at the Single-Atom Level

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• 作者：Patrick Steinegger ; Masato Asai ; Rugard Dressler ; Robert Eichler ; Yusuke Kaneya ; Akina Mitsukai ; Yuichiro Nagame ; Dave Piguet ; Tetsuya K. Sato ; Matthias Schädel ; Shinsaku Takeda ; Atsushi Toyoshima ; Kazuaki Tsukada ; Andreas Türler ; Alessio Vascon
• 刊名：Journal of Physical Chemistry C
• 出版年：2016
• 出版时间：April 7, 2016
• 年：2016
• 卷：120
• 期：13
• 页码：7122-7132
• 全文大小：652K
• ISSN：1932-7455

文摘

An isothermal vacuum chromatography setup for superheavy element chemistry studies was developed and tested online at the one-atom-at-a-time level. As a model system, the adsorption behavior of thallium on quartz was chosen with respect to a future chemical characterization of its superheavy homologue, element 113 (E113, Z = 113), using the described setup. Short-lived ¹⁸⁴Tl (t_1/2 = 10.1(5) s) was produced in the reaction ¹⁵²Gd(³⁵Cl, 3n)¹⁸⁴Tl and delivered as a mass-separated ion beam to the chemistry experiment: A subsurface implantation and a subsequent fast thermal release from a metal matrix was followed by isothermal vacuum chromatography as the chemical separation stage. Single atomic species passing this chromatographic separation were finally identified by time- and energy-resolved event-by-event α-spectroscopy using a diamond-based solid-state detector. The derived adsorption enthalpy of −ΔH_ads^SiO₂(Tl) = 158 ± 3 kJ·mol^–1 significantly exceeds available data but correlates well with the adsorption of other elements studied on the same surface. The described technique enables chemical experiments with short-lived transactinide elements (t_1/2 < 1 s), surpassing the rapidity of today’s state-of-the-art gas-phase experiments by at least 1 order of magnitude.