Yudai Shigekawa, Xiaojie Yin, Akihiro Nambu, Yang Wang, Hiromitsu Haba
To observe the $γ$ rays emitted from the low-lying isomeric state of $^{229}$Th ($^{229\rm{m}}$Th), we aim to dope fluoride crystals with its precursor $^{229}$Pa. In this study, we produced $^{229}$Pa by a 30-MeV proton bombardment on $^{232}$Th and developed a chemical separation method. The chemical yield of Pa was 93(4)%, and the physical production yield of $^{229}$Pa for the proton energy range of 29.0${-}$30.1 MeV was measured to be 9.4(8) MBq/${\rmμ}$Ah, which was more than 10 times higher than those of $^{232,230,228,233}$Pa. These high chemical and production yields will allow us to prepare fluoride crystals having a sufficient amount of $^{229}$Pa for the observation of the $γ$ rays of $^{229\rm{m}}$Th.
Kosuke Morita, Kouji Morimoto, Daiya Kaji, Hiromitsu Haba, Kazutaka Ozeki, Yuki Kudou, Takayuki Sumita, Yasuo Wakabayashi, Akira Yoneda, Kengo Tanaka, Sayaka Yamaki, Ryutaro Sakai, Takahiro Akiyama, Shin-ichi Goto, Hiroo Hasebe, Minghui Huang, Tianheng Huang, Eiji Ideguchi, Yoshitaka Kasamatsu, Kenji Katori, Yoshiki Kariya, Hidetoshi Kikunaga, Hiroyuki Koura, Hisaaki Kudo, Akihiro Mashiko, Keita Mayama, Shin-ichi Mitsuoka, Toru Moriya, Masashi Murakami, Hirohumi Murayama, Saori Namai, Akira Ozawa, Nozomi Sato, Keisuke Sueki, Mirei Takeyama, Fuyuki Tokanai, Takayuki Yamaguchi, Atsushi Yoshida
An isotope of the 113th element, i.e., 278[113], was produced in a nuclear reaction with a 70Zn beam on a 209Bi target. We observed six consecutive α-decays following the implantation of a heavy particle in nearly the same position in the semiconductor detector under an extremely low background condition. The fifth and sixth decays are fully consistent with the sequential decays of 262Db and 258Lr in both decay energies and decay times. This indicates that the present decay chain consisted of 278[113], 274Rg (Z=111), 270Mt (Z=109), 266Bh (Z=107), 262Db (Z=105), and 258Lr (Z=103) with firm connections. This result, together with previously reported results from 2004 and 2007, conclusively leads to the unambiguous production and identification of the isotope 278[113] of the 113th element.
Naohiko Otuka, Masayuki Aikawa, Sándor Takács, Damdinsuren Gantumur, Shuichiro Ebata, Lkhagvasuren Bold, Akihiro Nambu, Hiromitsu Haba
The isomeric ratios and cross sections were measured up to 50 MeV for production of $^{198m,g}$Au, $^{197m,g}$Hg, $^{195m,g}$Hg and other Hg, Au and Pt radionuclides in irradiation of natural platinum by alpha-particles using the stacked foil activation technique and offline gamma-ray spectrometry. The simultaneous decay curve analysis was applied to the emission rates of more than 40 gamma lines to directly derive the independent cross sections of all products without determining the cumulative cross sections. The measured cross sections and isomeric ratios were compared with those compiled in the EXFOR library and simulated by TALYS-2.0. We found that the $^{nat}$Pt($α$,x)198g+mAu, $^{197g+m}$Hg and $^{195g+m}$Hg cross sections are fairly reproduced by the simulation, while the simulation result requires adjustment of the spin cutoff parameter for better reproduction of the isomeric ratios.
Naohiko Otuka, Sandor Takacs, Masayuki Aikawa, Shuichiro Ebata, Hiromitsu Haba
The isomeric ratios of $^{198}$Au, $^{197}$Hg and $^{195}$Hg produced by $α$-particle induced reactions on natural platinum were investigated experimentally up to 29 MeV by using the standard stacked foil activation technique and $γ$-ray spectrometry. The isomeric ratios of $^{197}$Hg and $^{195}$Hg determined by the conventional activation cross section formula showed strong cooling time dependence. The time dependence was resolved by adjusting the isomeric transition branching ratios for the two isotopes within a simultaneous decay curve analysis framework. Our analysis suggests 94.5$\pm$0.7% and 48.9$\pm$1.8% as the isomeric transition branching ratios of $^{197m}$Hg (24 h) and $^{195m}$Hg (42 h), respectively. The isomeric ratios and independent production cross sections of $^{198}$Au, $^{197}$Hg, $^{195}$Hg and some other Hg, Au and Pt isotopes were also measured down to 6 MeV with these corrected isomeric transition branching ratios, and compared with predictions of statistical and pre-equilibrium models by TALYS-2.0 to discuss spin cuto? parameter dependence. We found the measured isomeric ratios are better predicted if we reduce the spin cuto? parameter to half or less from that estimated with the rigid body moment of inertia.
Yamato Fujii, Naohiko Otuka, Kenta Sugihara, Masayuki Aikawa, Hiromitsu Haba, Isao Murata
The influence of the secondary neutrons on measurements of alpha-particle activation cross sections below the Coulomb barrier was studied for the $^\mathrm{nat}$Pt($α$,x)$^\mathrm{195m}$Pt reaction. We characterized the secondary neutron field by using the particle transport simulation code PHITS, and estimated the $^\mathrm{nat}$Pt(n,x)$^\mathrm{195m}$Pt yields by using the characterized neutron spectra and the $^\mathrm{nat}$Pt(n,x)$^{195m}$Pt cross sections in the JENDL-5/A library. We confirmed that the unexpectedly high $^\mathrm{nat}$Pt($α$,x)$^\mathrm{195m}$Pt cross sections below the Coulomb barrier measured by us are explained well by the $^\mathrm{nat}$Pt(n,x)$^\mathrm{195m}$Pt reaction induced by the secondary neutrons. This indicates that the secondary neutron effect is sometimes not negligible even in low energy charged-particle activation cross section measurements. We also studied the influence of the secondary light charged particles by the same approach, and confirmed that their influence is negligible.
Sota Kimura, Michiharu Wada, Hiromitsu Haba, Hironobu Ishiyama, Toshitaka Niwase, Marco Rosenbusch, Peter Schury
The influence of isotope differences on ion charge state yield ratios has never been studied in detail, having been considered negligible. However, we have observed anomalous ion charge state distributions in the thermalization of energetic atomic ions in helium gas; the charge state distributions varied between not only isotopes but also between nuclear states within the same nuclide. The magnitude of the observed results suggests that this anomaly is a universal phenomenon that cannot be explained by the framework of the known isotope effects. Nuclear spin and deformation could be key to unraveling this, but the mechanisms remain an open question.
Sota Kimura, Michiharu Wada, Hiromitsu Haba, Hironobu Ishiyama, Satoshi Ishizawa, Yuta Ito, Toshitaka Niwase, Marco Rosenbusch, Peter Schury, Aiko Takamine
We report the mass measurements of neutron-rich isotopes produced via spontaneous fission of ${}^{252}$Cf using a multi-reflection time-of-flight mass spectrograph. The mass of ${}^{155}$Ce is determined experimentally for the first time. A discrepancy between the experimental and literature values was found for the mass of ${}^{127}$Sb, which was previously deduced through indirect measurements. In comparison with several theoretical predictions, both the values and the trend of the mass excesses of ${}^{152-155}$Ce cannot be consistently explained. The wide-range and simultaneous mass measurements of the multi-reflection time-of-flight mass spectrograph enable us to cross-check the existing mass data, and the conflict between the measured time-of-flight ratio and the extracted mass would imply the necessity of reexamining them.
Tomonori Fukuchi, Mika Shigeta, Hiromitsu Haba, Daiki Mori, Takuya Yokokita, Yukiko Komori, Seiichi Yamamoto, Yasuyoshi Watanabe
We developed a positron emission tomography (PET) system for multiple-isotope imaging. Our PET system, named multiple-isotope PET (MI-PET), can distinguish between different tracer nuclides using coincidence measurement of prompt gamma-rays, which are emitted after positron emission. In MI-PET imaging with a pure positron emitter and prompt-gamma emitter, because of the imperfectness of prompt gamma-ray detection, an image for a pure positron emitter taken by MI-PET is superposed by a positron-γ emitter. Therefore, in order to make isolated images of the pure positron emitter, we developed image reconstruction methods based on data subtraction specific to MI-PET. We tested two methods, subtraction between reconstructed images and subtraction between sinogram data. In both methods, normalization for position dependence of the prompt γ-ray sensitivity is required in addition to detector sensitivity normalization. For these normalizations, we performed normalization scans using cylindrical phantoms of the positron-gamma emitters Sc-44m and Na-22. A long period measurement using the activity decay of Sc-44m (Half-life 58.6 hours) elucidated that the acquisition ratio between the prompt gamma-rays coincided with PET event and pure PET event changes on the basis of object activities. Therefore, we developed a correction method that involves subtraction parameters dependent on the activities, i.e., the counting rate. From analysis of dual-tracer phantom images, data subtraction in the sinogram data with sensitivity correction gives a higher quality of isolated images for the pure positron emitter than those from image subtractions. Furthermore, from dual-isotope (F-18-FDG and Sc-44m) mouse imaging, we concluded that our developed method can be used for practical imaging of a living organism.
Takahiro Hiraki, Koichi Okai, Michael Bartokos, Kjeld Beeks, Hiroyuki Fujimoto, Yuta Fukunaga, Hiromitsu Haba, Yoshitaka Kasamatsu, Shinji Kitao, Adrian Leitner, Takahiko Masuda, Guan Ming, Nobumoto Nagasawa, Ryoichiro Ogake, Martin Pimon, Martin Pressler, Noboru Sasao, Fabian Schaden, Thorsten Schumm, Makoto Seto, Yudai Shigekawa, Koutaro Shimizu, Tomas Sikorsky, Kenji Tamasaku, Sayuri Takatori, Tsukasa Watanabe, Atsushi Yamaguchi, Yoshitaka Yoda, Akihiro Yoshimi, Koji Yoshimura
The radioisotope Th-229 is renowned for its extraordinarily low-energy, long-lived nuclear first-excited state. This isomeric state can be excited by VUV lasers and the transition from the ground state has been proposed as a reference transition for ultra-precise nuclear clocks. Such nuclear clocks will find multiple applications, ranging from fundamental physics studies to practical implementations. Recent investigations extracted valuable constraints on the nuclear transition energy and lifetime, populating the isomer in stochastic nuclear decay of U-233 or Ac-229. However, to assess the feasibility and performance of the (solid-state) nuclear clock concept, time-controlled excitation and depopulation of the $^{229}$Th isomer together with time-resolved monitoring of the radiative decay are imperative. Here we report the population of the $^{229}$Th isomeric state through resonant X-ray pumping and detection of the radiative decay in a VUV transparent $^{229}$Th-doped CaF$_2$ crystal. The decay half-life is measured to $447\pm 25$ s, with a transition wavelength of $148.18 \pm 0.42$ 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 by at least a factor 50. Such controlled quenching can be used to significantly speed up the interrogation cycle in future nuclear clock schemes. Our results show that full control over the $^{229}$Th nuclear isomer population can be achieved in a crystal environment. In particular, non-radiative decay processes that might lead to a broadening of the isomer transition linewidth are negligible, paving the way for the development of a compact and robust solid-state nuclear clock. Further studies are needed to reveal the underlying physical mechanism of the X-ray quenching effect.
Ming Guan, Michael Bartokos, Kjeld Beeks, Hiroyuki Fujimoto, Yuta Fukunaga, Hiromitsu Haba, Takahiro Hiraki, Yoshitaka Kasamatsu, Shinji Kitao, Adrian Leitner, Takahiko Masuda, Nobumoto Nagasawa, Koichi Okai, Ryoichiro Ogake, Martin Pimon, Martin Pressler, Noboru Sasao, Fabian Schaden, Thorsten Schumm, Makoto Seto, Yudai Shigekawa, Kotaro Shimizu, Tomas Sikorsky, Kenji Tamasaku, Sayuri Takatori, Tsukasa Watanabe, Atsushi Yamaguchi, Yoshitaka Yoda, Akihiro Yoshimi, Koji Yoshimura
Thorium-229 has the lowest nuclear-excited state (an isomer state) at approximately 8.356 eV, making it excitable with tabletop vacuum-ultraviolet lasers. Despite the recent success of laser excitation, the isomer quenching inside the solid-state environment remains unresolved. In this letter, we present experiments investigating X-ray-induced isomer quenching in the CaF$_2$ host, focusing on the effects of X-ray flux and temperature on the lifetime and yield of the isomer state. Our studies reveal a correlation between isomer production, isomer lifetime during irradiation, and post-irradiation afterglow of the target crystal across different temperatures, highlighting a strong relationship between isomer quenching and color-center dynamics. We developed a model to interpret the isomer quenching and the crystal's luminescence.
Masayuki Aikawa, Moemi Saito, Shuichiro Ebata, Yukiko Komori, Hiromitsu Haba
The production cross sections of $^{68,69}$Ge and $^{66,67}$Ga by α-induced reactions on $^{nat}$Zn have been measured using the stacked-foil activation method and off-line γ-ray spectrometry from their threshold energies to 50.7 MeV. The derived cross sections were compared with the previous experimental data and the calculated values in the TENLD-2017 library. Our result shows a slightly larger amplitude than the previous data at the peak, though the peak energy is consistent with them.
Takahiko Masuda, Akihiro Yoshimi, Akira Fujieda, Hiroyuki Fujimoto, Hiromitsu Haba, Hideaki Hara, Takahiro Hiraki, Hiroyuki Kaino, Yoshitaka Kasamatsu, Shinji Kitao, Kenji Konashi, Yuki Miyamoto, Koichi Okai, Sho Okubo, Noboru Sasao, Makoto Seto, Thorsten Schumm, Yudai Shigekawa, Kenta Suzuki, Simon Stellmer, Kenji Tamasaku, Satoshi Uetake, Makoto Watanabe, Tsukasa Watanabe, Yuki Yasuda, Atsushi Yamaguchi, Yoshitaka Yoda, Takuya Yokokita, Motohiko Yoshimura, Koji Yoshimura
Thorium-229 is a unique case in nuclear physics: it presents a metastable first excited state Th-229m, just a few electronvolts above the nuclear ground state. This so-called isomer is accessible by VUV lasers, which allows transferring the amazing precision of atomic laser spectroscopy to nuclear physics. Being able to manipulate the Th-229 nuclear states at will opens up a multitude of prospects, from studies of the fundamental interactions in physics to applications as a compact and robust nuclear clock. However, direct optical excitation of the isomer or its radiative decay back to the ground state has not yet been observed, and a series of key nuclear structure parameters such as the exact energies and half-lives of the low-lying nuclear levels of Th-229 are yet unknown. Here we present the first active optical pumping into Th-229m. Our scheme employs narrow-band 29 keV synchrotron radiation to resonantly excite the second excited state, which then predominantly decays into the isomer. We determine the resonance energy with 0.07 eV accuracy, measure a half-life of 82.2 ps, an excitation linewidth of 1.70 neV, and extract the branching ratio of the second excited state into the ground and isomeric state respectively. These measurements allow us to re-evaluate gamma spectroscopy data that have been collected over 40~years.