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1.
Nature ; 573(7773): 238-242, 2019 09.
Artículo en Inglés | MEDLINE | ID: mdl-31511686

RESUMEN

The metastable first excited state of thorium-229, 229mTh, is just a few electronvolts above the nuclear ground state1-4 and is accessible by vacuum ultraviolet lasers. The ability to manipulate the 229Th nuclear states with the precision of atomic laser spectroscopy5 opens up several prospects6, from studies of fundamental interactions in physics7,8 to applications such as a compact and robust nuclear clock5,9,10. However, direct optical excitation of the isomer and its radiative decay to the ground state have not yet been observed, and several key nuclear structure parameters-such as the exact energies and half-lives of the low-lying nuclear levels of 229Th-remain unknown11. Here we present active optical pumping into 229mTh, achieved using narrow-band 29-kiloelectronvolt synchrotron radiation to resonantly excite the second excited state of 229Th, which then decays predominantly into the isomer. We determine the resonance energy with an accuracy of 0.07 electronvolts, measure a half-life of 82.2 picoseconds and an excitation linewidth of 1.70 nanoelectronvolts, and extract the branching ratio of the second excited state into the ground and isomeric state. These measurements allow us to constrain the 229mTh isomer energy by combining them with γ-spectroscopy data collected over the past 40 years.

2.
J Phys Chem A ; 128(14): 2717-2726, 2024 Apr 11.
Artículo en Inglés | MEDLINE | ID: mdl-38563068

RESUMEN

The hydration structure of No2+, the divalent cation of nobelium in water, was investigated by ab initio molecular dynamics (MD) simulations. First, a series of benchmark calculations were performed to validate the density functional theory (DFT) calculation methods for a molecule containing a No atom. The DFT-MD simulation of the hydration structure of No2+ was conducted after the MD method was validated by simulating the hydration structures of Ca2+ and Sr2+, whose behavior was previously reported to be similar to that of No2+. The model cluster containing M2+ (M = Ca, Sr, or No) and 32 water molecules was used for DFT-MD simulation. The results showed that the hydration distance of No2+ was intermediate between those of Ca2+ and Sr2+. This trend in the hydration distance is in good agreement with the elution position trend obtained in a previous radiochemical experiment. The calculated No-O bond lengths in the optimized structure of [No(H2O)8]2+ was 2.59 Å, while the average No-O bond length of [No(H2O)8]2+ in water by DFT-MD was 2.55 Å. This difference implies the importance of dynamic solvent effects, considering the second (and further) coordination sphere in the theoretical calculation of solution chemistry for superheavy elements.

3.
Nat Commun ; 15(1): 5536, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-39013899

RESUMEN

The radioisotope thorium-229 (229Th) is renowned for its extraordinarily low-energy, long-lived nuclear first-excited state. This isomeric state can be excited by vacuum ultraviolet (VUV) lasers and 229Th has been proposed as a reference transition for ultra-precise nuclear clocks. To assess the feasibility and performance of the nuclear clock concept, time-controlled excitation and depopulation of the 229Th isomer are imperative. Here we report the population of the 229Th isomeric state through resonant X-ray pumping and detection of the radiative decay in a VUV transparent 229Th-doped CaF2 crystal. The decay half-life is measured to 447(25) s, with a transition wavelength of 148.18(42) nm and a radiative decay fraction consistent with unity. Furthermore, we report a new "X-ray quenching" effect which allows to de-populate the isomer on demand and effectively reduce the half-life. Such controlled quenching can be used to significantly speed up the interrogation cycle in future nuclear clock schemes.

4.
Inorg Chem ; 52(21): 12311-3, 2013 Nov 04.
Artículo en Inglés | MEDLINE | ID: mdl-24116851

RESUMEN

The reduction behavior of mendelevium (Md) was studied using a flow electrolytic chromatography apparatus. By application of the appropriate potentials on the chromatography column, the more stable Md(3+) is reduced to Md(2+). The reduction potential of the Md(3+) + e(-) → Md(2+) couple was determined to be -0.16 ± 0.05 V versus a normal hydrogen electrode.

5.
Appl Radiat Isot ; 179: 110006, 2022 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-34768147

RESUMEN

For new chemical studies on heavy elements, we previously investigated the coprecipitation behaviors with samarium hydroxide for various elements. Herein, we report the coprecipitation experiment using multitracer produced by neutron-induced fission of 235U. The coprecipitation behaviors of 10 elements were investigated: new data were obtained for Sr, Ru, I, Pm, and Np. The present results support the previously obtained conclusion that the hydroxide precipitation properties of various elements can be qualitatively investigated through their coprecipitation behaviors.

6.
Nat Chem ; 13(3): 226-230, 2021 03.
Artículo en Inglés | MEDLINE | ID: mdl-33589784

RESUMEN

All superheavy elements (SHEs), with atomic numbers (Z) ≥104, have been artificially synthesized one atom at a time and their chemical properties are largely unknown. Because these heavy nuclei have short lifetimes as well as extremely low production rates, chemical experiments need to be carried out on single atoms and have mostly been limited to adsorption and extraction. We have now investigated the precipitation properties of the SHE Rf (Z = 104). A co-precipitation method with samarium hydroxide had previously established that the co-precipitation behaviour of a range of elements reflected these elements' tendency to form hydroxide precipitates and/or ammine complex ions. Here we investigated co-precipitation of Rf in basic solutions containing NH3 or NaOH. Comparisons between the behaviour of Rf with that of Zr and Hf (lighter homologues of Rf) and actinide Th (a pseudo-homologue of Rf) showed that Rf does not coordinate strongly with NH3, but forms a hydroxide (co)precipitate that is expected to be Rf(OH)4.

7.
J Am Chem Soc ; 131(26): 9180-1, 2009 Jul 08.
Artículo en Inglés | MEDLINE | ID: mdl-19514720

RESUMEN

We report here on the successful oxidation of element 102, nobelium (No), on an atom-at-a-time scale in 0.1 M alpha-hydroxyisobutyric acid (alpha-HIB) solution using a newly developed technique, flow electrolytic column chromatography. It is found that the most stable ion, No(2+), is oxidized to No(3+) within 3 min and that the oxidized No complex with alpha-HIB holds the trivalent state in the column above an applied potential of 1.0 V.

8.
Appl Radiat Isot ; 66(3): 271-7, 2008 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-17826145

RESUMEN

We have developed a new target-irradiation system for the online preparation of multitracer solutions, where the nuclear-reaction products recoiling out of the target are directly implanted in a solvent as a liquid catcher. A rapid online transportation of the solution has enabled highly efficient recovery of the multitracer solutions having even short-lived radioactive isotopes without any chemical treatments. It has been suggested that the collection efficiency depends on the chemical properties of the recoil elements.

9.
Appl Radiat Isot ; 118: 105-116, 2016 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-27623042

RESUMEN

To establish a new methodology for superheavy element chemistry, the coprecipitation behaviors of 34 elements with samarium hydroxide were investigated using multitracer produced by a spallation of Ta. The chemical reactions were rapidly equilibrated within 10s for many elements. In addition, these elements exhibited individual coprecipitation behaviors, and the behaviors were qualitatively related to their hydroxide precipitation behaviors. It was demonstrated that the ammine and hydroxide complex formations of superheavy elements could be investigated using the established method.

10.
Dalton Trans ; 45(47): 18827-18831, 2016 Nov 29.
Artículo en Inglés | MEDLINE | ID: mdl-27853791

RESUMEN

We successfully observed the equilibrium state of the chemical reactions for superheavy elements on a one-atom-at-a-time scale; we investigated the time dependence of the extraction behaviour of element 104, Rf. The distribution coefficient of Rf in 9 M HCl was found to be higher than those of its homologous elements, probably due to differences in the chloride complexation of Rf.

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