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Journal Articles

First ionization potentials of Fm, Md, No, and Lr; Verification of filling-up of 5f electrons and confirmation of the actinide series

Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Beerwerth, R.*; Kaneya, Yusuke*; Makii, Hiroyuki; Mitsukai, Akina*; Nagame, Yuichiro; Osa, Akihiko; Toyoshima, Atsushi; et al.

Journal of the American Chemical Society, 140(44), p.14609 - 14613, 2018/11

 Times Cited Count:29 Percentile:69.01(Chemistry, Multidisciplinary)

The first ionization potential (IP$$_1$$) yields information on valence electronic structure of an atom. IP$$_1$$ values of heavy actinides beyond einsteinium (Es, Z = 99), however, have not been determined experimentally so far due to the difficulty in obtaining these elements on scales of more than one atom at a time. Recently, we successfully measured IP$$_1$$ of lawrencium (Lr, Z = 103) using a surface ionization method. The result suggests that Lr has a loosely-bound electron in the outermost orbital. In contrast to Lr, nobelium (No, Z = 102) is expected to have the highest IP$$_1$$ among the actinide elements owing to its full-filled 5f and the 7s orbitals. In the present study, we have successfully determined IP$$_1$$ values of No as well as fermium (Fm, Z = 100) and mendelevium (Md, Z = 101) using the surface ionization method. The obtained results indicate that the IP$$_1$$ value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.

Journal Articles

Measurement of the first ionization potential of lawrencium by surface ionization method

Sato, Tetsuya

Genshikaku Kenkyu, 61(1), p.96 - 106, 2016/09

We successfully determined the first ionization potential of lawrencium (Lr, Z=103). The result experimentally substantiated for the first time that Lr is the last member of the actinide series. Measured ionization potential suggested that Lr atom would have the electronic configuration which is different from the configuration expected based on the Periodic table. For the measurement, we have developed a novel method applied the surface ionization process. Public responses after the publication are also introduced.

Journal Articles

Does element-103 change the periodic table of elements ?!; The First ionization potential of lawrencium

Sato, Tetsuya

Kagaku, 71(3), p.12 - 16, 2016/03

We successfully confirmed that lawrencium, element 103, would be the last member of actinide series by a measurement of the first ionization potential of lawrencium. Moreover, the electronic configuration expected from the experimental results suggested that lawrencium could have the outermost electronic orbital similar to that of group-13 elements. Our result triggered discussion concerning the position of lawrencium and lutetium on the periodic table of the elements.

Journal Articles

The First ionization potential of element 103 successfully measured for the first time substantiated that lawrencium is the last member of actinide series

Sato, Tetsuya

Isotope News, (740), p.16 - 19, 2015/12

We successfully determined the first ionization potential of lawrencium (Lr, Z=103). The result experimentally substantiated for the first time that Lr is the last member of the actinide series. Measured ionization potential suggested that Lr atom would have the electronic configuration which is different from the configuration expected based on the Periodic table.

Journal Articles

Measurement of the first ionization energy of lawrencium (Z = 103) by surface ionization technique

Sato, Tetsuya

Hosha Kagaku, (32), p.34 - 41, 2015/09

In the surface ionization process, an ionization efficiency depends on the first ionization potential of the atom of the element. The ionization potential can be estimated by using the relationship. This method has been developed in order to determine the first ionization potential of lawrencium (Lr, element 103). The value of the ionization potential of Lr have not been measured experimentally due to its low production rate and short half-life. The surface-ionization method is described in detail in this paper.

Journal Articles

Measurement of the first ionization potential of lawrencium, element 103

Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Stora, T.*; Sato, Nozomi; Kaneya, Yusuke; Tsukada, Kazuaki; D$"u$llmann, Ch. E.*; Eberhardt, K.*; Eliav, E.*; et al.

Nature, 520(7546), p.209 - 211, 2015/04

 Times Cited Count:109 Percentile:97.59(Multidisciplinary Sciences)

Ionization efficiency in a surface ionization process depends on the first ionization potential of the atom. Based on the dependence, the ionization potential of the atom can be determined. We successfully measured ionization efficiencies of lawrencium (Lr, $$Z$$=103) using a gas-jet coupled surface ion-source. The ionization potential of Lr has not been determined owing to its low production rate and its short half-life. Based on a relationship between the ionization efficiency and the ionization potential obtained via measurements of short-lived lanthanide isotopes, the ionization potential of Lr was determined.

Oral presentation

First ionization energy measurements of heaviest actinides, lawrencium and nobelium

Sato, Tetsuya

no journal, , 

We measured the first ionization energy (IE$$_1$$) of nobelium (No, Z = 102) and lawrencium (Lr, Z =103) by exploiting the dependence of the ionization efficiency ($$I_{rm eff}$$) on the IE$$_1$$ in a surface ionization process. The isotopes $$^{257}$$No ($$T_{1/2}$$ = 24.5s) and $$^{256}$$Lr ($$T_{1/2}$$ = 27 s), produced in the reaction $$^{248}$$Cm ($$^{13}$$C, 4n) and $$^{249}$$Cf ($$^{11}$$B, 4n), respectively, were used for studying their ionization. The reaction products recoiling from the targets were transported to a surface ion-source by a He/CdI$$_2$$ gas-jet transport system. The products ionized in the ion-source were mass-separated with JAEA-ISOL. The number of ions collected at the end of the ISOL was determined by $$alpha$$-particle measurements and was used to evaluate $$I_{rm eff}$$ values. With the present system, we successfully ionized and mass-separated $$^{257}$$No and $$^{256}$$Lr with efficiencies of (0.5 $$pm$$ 0.1)% and (36 $$pm$$ 7)% at 2800 K, respectively. From these $$I_{rm eff}$$ values, IE$$_1$$ values of No and Lr were determined based on the relationship between $$I_{rm eff}$$ and IE$$_1$$. Our values are in good agreement with the predicted ones by theoretical calculations.

Oral presentation

First ionization potentials of heavy actinides

Sato, Tetsuya; Asai, Masato; Kaneya, Yusuke*; Tsukada, Kazuaki; Toyoshima, Atsushi; Mitsukai, Akina*; Takeda, Shinsaku*; Vascon, A.*; Sakama, Minoru*; Sato, Daisuke*; et al.

no journal, , 

The first ionization potential (IP$$_1$$) yields information on valence electronic structure of an atom. IP$$_1$$ values of heavy actinides beyond einsteinium (Es, Z = 99), however, have not been determined experimentally so far due to the difficulty in obtaining these elements on scales of more than one atom at a time. Recently, we successfully measured IP$$_1$$ of lawrencium (Lr, Z = 103) using a surface ionization method. The result suggests that Lr has a loosely-bound electron in the outermost orbital. In contrast to Lr, nobelium (No, Z = 102) is expected to have the highest IP$$_1$$ among the actinide elements owing to its full-filled 5f and the 7s orbitals. In the present study, we have successfully determined IP$$_1$$ values of No as well as fermium (Fm, Z = 100) and mendelevium (Md, Z = 101) using the surface ionization method. The obtained results indicate that the IP$$_1$$ value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.

Oral presentation

Discrepancy in the periodic table appears at element 103; The Periodic table of elements might be restructured

Sato, Tetsuya

no journal, , 

The first ionization potential (IP$$_1$$) of element 103, lawrencium (Lr), has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP$$_1$$ value is 4.96 $$pm$$ 0.08 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15) eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]$$7s^25f^{14}7p_{1/2}$$, which is influenced by strong relativistic effects. The present work opens the way for studies on atomic properties of heavy elements with atomic number $$Z > 100$$. Moreover, the present achievement has triggered a controversy on the position of lutetium (Lu) and Lr in the Periodic Table of Elements.

Oral presentation

Ionization potential measurements of the heaviest actinides

Sato, Tetsuya

no journal, , 

The first ionization potential (IP$$_1$$) yields information on valence electronic structure of an atom. IP$$_1$$ values of heavy actinides beyond einsteinium (Es, Z = 99), however, have not been determined experimentally so far due to the difficulty in obtaining these elements on scales of more than one atom at a time. Recently, we successfully measured IP$$_1$$ of lawrencium (Lr, Z = 103) using a surface ionization method. In the present study, we have successfully determined IP$$_1$$ values of No as well as fermium (Fm, Z = 100) and mendelevium (Md, Z = 101) using the surface ionization method. The obtained results indicate that the IP$$_1$$ value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.

Oral presentation

Measurements of the first ionization potentials of heavy actinides

Sato, Tetsuya; Asai, Masato; Kaneya, Yusuke*; Tsukada, Kazuaki; Toyoshima, Atsushi; Mitsukai, Akina*; Takeda, Shinsaku*; Vascon, A.*; Sakama, Minoru*; Sato, Daisuke*; et al.

no journal, , 

The first ionization potential (IP$$_1$$) yields information on valence electronic structure of an atom. IP$$_1$$ values of heavy actinides beyond einsteinium (Es, Z = 99), however, have not been determined experimentally so far due to the difficulty in obtaining these elements on scales of more than one atom at a time. Recently, we successfully measured IP$$_1$$ of lawrencium (Lr, Z = 103) using a surface ionization method. The result suggests that Lr has a loosely-bound electron in the outermost orbital. In contrast to Lr, nobelium (No, Z = 102) is expected to have the highest IP$$_1$$ among the actinide elements owing to its full-filled 5f and the 7s orbitals. In the present study, we have successfully determined IP$$_1$$ values of No as well as fermium (Fm, Z = 100) and mendelevium (Md, Z = 101) using the surface ionization method. The obtained results indicate that the IP$$_1$$ value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.

Oral presentation

Measurements of the first ionization potentials of heavy actinide elements

Sato, Tetsuya

no journal, , 

The first ionization potential (IP$$_1$$), a measure of the energy required to remove one valence electron from a neutral atom, yields information on the valence electronic structure. Recently, we successfully determined the IP$$_1$$ value of the heaviest actinide element, lawrencium (Lr, $$Z = 103$$) for the first time in an atom-at-a-time scale using a surface ionization method. The experimental result has shown that the IP$$_1$$ of Lr is distinctly low among actinide elements owing to the configuration of closed $$5f^{14}$$ and $$7s^2$$ shells with an additional weakly-bound electron in the valence orbital. As a next step, we have applied this method to IP$$_1$$ measurements of other heavy actinide elements, No, mendelevium (Md, $$Z = 101$$) and fermium (Fm, $$Z = 100$$). The experimental results of the three elements are in good agreement with the predicted ones obtained by theoretical and/or semi-empirical calculations. The IP$$_1$$ value increased with an atomic number up to No and fell dramatically at Lr, indicating the similar trend with that of heavy lanthanide elements. This behavior clearly indicates that the $$5f$$ orbital is filled up at No.

Oral presentation

Atomic/chemical properties of the heaviest actinide element lawrencium

Sato, Tetsuya

no journal, , 

In order to discuss the chemical and atomic properties of heavy elements with atomic numbers greater than 100 which are affected by strong relativistic effects, we successfully determined the first ionization potential (IP$$_1$$) value of the heaviest actinide element, lawrencium (Lr, $$Z$$ = 103) on scales of one atom at a time by using a surface ion-source installed in the Isotope Separator On-Line (ISOL) at the JAEA tandem accelerator. In addition, we conducted to observe adsorption-desorption behavior of Lr atom on tantalum surface using similar set-up. The results suggested that Lr would have a $$7p_{1/2}$$ orbital as the outermost electronic one and a low volatility like lutetium, the lanthanide homologue of Lr.

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