TY - JOUR
T1 - Vacuum Chromatography of Tl on SiO2 at the Single-Atom Level
AU - Steinegger, Patrick
AU - Asai, Masato
AU - Dressler, Rugard
AU - Eichler, Robert
AU - Kaneya, Yusuke
AU - Mitsukai, Akina
AU - Nagame, Yuichiro
AU - Piguet, Dave
AU - Sato, Tetsuya K.
AU - Schädel, Matthias
AU - Takeda, Shinsaku
AU - Toyoshima, Atsushi
AU - Tsukada, Kazuaki
AU - Türler, Andreas
AU - Vascon, Alessio
N1 - Funding Information:
This project is supported by the Swiss National Science Foundation (grant: 200020-144511) and CIVIDEC Instrumentation GmbH.
Publisher Copyright:
© 2016 American Chemical Society.
PY - 2016/4/7
Y1 - 2016/4/7
N2 - 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 (t1/2 = 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 -ΔHadsSiO2(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 (t1/2 < 1 s), surpassing the rapidity of today's state-of-the-art gas-phase experiments by at least 1 order of magnitude. (Figure Presented).
AB - 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 (t1/2 = 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 -ΔHadsSiO2(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 (t1/2 < 1 s), surpassing the rapidity of today's state-of-the-art gas-phase experiments by at least 1 order of magnitude. (Figure Presented).
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U2 - 10.1021/acs.jpcc.5b12033
DO - 10.1021/acs.jpcc.5b12033
M3 - Article
AN - SCOPUS:84964325580
SN - 1932-7447
VL - 120
SP - 7122
EP - 7132
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 13
ER -