Bromine-isotope selective ionization using field-free alignment of IBr isotopologues with a switched nanosecond laser pulse

Akagi, Hiroshi*; Kumada, Takayuki; Otobe, Tomohito*; Itakura, Ryuji*; Hasegawa, Hirokazu*; Oshima, Yasuhiro*

Chemistry Letters, 49(4), p.416 - 418, 2020/04

https://doi.org/10.1246/cl.200024

Isotope-selective ionization utilizing field-free alignment of isotopologues using a switched nanosecond laser pulse

Akagi, Hiroshi*; Kumada, Takayuki; Otobe, Tomohito*; Itakura, Ryuji*; Hasegawa, Hirokazu*; Oshima, Yasuhiro*

Applied Physics B, 124(1), p.14_1 - 14_8, 2018/01

https://doi.org/10.1007/s00340-017-6884-7

We propose and numerically simulate a method of laser isotope separation based on field-free alignment of isotopologues, utilizing an intense switched nanosecond (ns) laser field which is slowly turned on and rapidly turned off at the peak with the falling time of 200 fs. The femtosecond (fs) laser induced alignment of molecules including a heavy atom is severely disturbed by ionization because of their small ionization potential. Our simulations for IBr and IBr isotopologues demonstrate that the switched ns laser field can make isotopologues well-aligned with the reduced ionization probability at the laser intensity which is an order-of-magnitude lower than a typical intensity for field-free alignment induced by a fs laser field.

Complex chemistry with complex compounds

Eichler, R.*; Asai, Masato; Brand, H.*; Chiera, N. M.*; Di Nitto, A.*; Dressler, R.*; Dllmann, Ch. E.*; Even, J.*; Fangli, F.*; Goetz, M.*; et al.

EPJ Web of Conferences, 131, p.07005_1 - 07005_7, 2016/12

https://doi.org/10.1051/epjconf/201613107005

In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the productions and investigations of fragile single molecular species of superheavy elements. The latest highlight is the formation of very volatile hexacarbonyl compound of element 106, Sg(CO). Following this success, second-generation experiments were performed to measure the first bond dissociation energy between the central metal atom and the surrounding ligand. The method using a tubular decomposition reactor was developed and successfully applied to short-lived Mo(CO), W(CO), and Sg(CO).

Decomposition studies of group 6 hexacarbonyl complexes, 1; Production and decomposition of Mo(CO) and W(CO)

Usoltsev, I.*; Eichler, R.*; Wang, Y.*; Even, J.*; Yakushev, A.*; Haba, Hiromitsu*; Asai, Masato; Brand, H.*; Di Nitto, A.*; Dllmann, Ch. E.*; et al.

Radiochimica Acta, 104(3), p.141 - 151, 2016/03

https://doi.org/10.1515/ract-2015-2445

Conditions of the production and decomposition of hexacarbonyl complexes of short-lived Mo and W isotopes were investigated to study thermal stability of the heaviest group 6 hexacarbonyl complex Sg(CO). A tubular flow reactor was tested to decompose the hexacarbonyl complexes and to extract the first bond dissociation energies. A silver was found to be the most appropriate reaction surface to study the decomposition of the group 6 hexacarbonyl. It was found that the surface temperature at which the decomposition occurred was correlated to the first bond dissociation energy of Mo(CO) and W(CO), indicating that the first bond dissociation energy of Sg(CO) could be determined with this technique.

Investigation of an excavation damaged zone in the east access shaft at the Horonobe Underground Research Laboratory

Aoyagi, Kazuhei; Ishii, Eiichi; Fujita, Tomoo; Motoshima, Takayuki*

Dai-44-Kai Gamban Rikigaku Ni Kansuru Shimpojiumu Koenshu (CD-ROM), p.313 - 318, 2016/01

The objective of this research is to investigate the extent and failure mechanism of an Excavation Damaged Zone (EDZ) induced around the East Access Shaft in the Horonobe Underground Research Laboratory. As a result of hydraulic tests, hydraulic conductivity within 2 m from the shaft wall was increased by 1 to 3 orders of magnitude. This result is consistent with the extent of the development of fractures detected by borehole televiewer surveys. Furthermore, the dominant failure mechanism of the fractures around the shaft wall was almost tensile; also these fractures were caused by the short-term excavation-induced unloading.

Isotope-selective ionization utilizing field-free alignment of isotopologues with a train of femtosecond laser pulses

Akagi, Hiroshi; Kasajima, Tatsuya*; Kumada, Takayuki; Itakura, Ryuji; Yokoyama, Atsushi; Hasegawa, Hirokazu*; Oshima, Yasuhiro*

Physical Review A, 91(6), p.063416_1 - 063416_7, 2015/06

https://doi.org/10.1103/PhysRevA.91.063416

We propose a strategy of isotope-selective ionization for a binary mixture of isotopologues of homonuclear diatomic molecules, utilizing field-free alignment with a train of femtosecond laser pulses. Field-free alignment can be achieved simultaneously for two isotopologues consisting of two atoms with the same atomic mass number or , utilizing a pulse train with their time interval of T = T() = T(), where T() and T() are the rotational revival times of the isotopologues. We demonstrate experimentally that a train of four alignment pulses with their interval of T ( = 14, = 15) creates transiently aligned N and anti-aligned N just before T/2 after the last pulse, and vice versa just after T/2. Highly isotope-selective N ionization is achieved at these timings with another femtosecond laser pulse, which induces the non-resonant multiphoton ionization with the cross section remarkably depending on the angle between the molecular axis and the laser electric field direction. The ion yield ratio I(N)/I(N) ranges from 0.49 to 2.00, which is wider than the range obtained with single alignment pulse.

In situ synthesis of volatile carbonyl complexes with short-lived nuclides

Even, J.*; Ackermann, D.*; Asai, Masato; Block, M.*; Brand, H.*; Di Nitto, A.*; Dllmann, Ch. E.*; Eichler, R.*; Fan, F.*; Haba, Hiromitsu*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 303(3), p.2457 - 2466, 2015/03

https://doi.org/10.1007/s10967-014-3793-7

Rapid In situ synthesis of metal carbonyl complexes has been demonstrated using short-lived isotopes produced in nuclear fission and fusion reactions. The short-lived isotopes with high recoil energy directly react with carbon-monoxides and form carbonyl complexes. Only highly volatile complexes were fast transported in a gas stream to counting and chemistry devices. Short-lived Mo, Tc, Ru, Rh, W, Re, Os, and Ir were found to form volatile carbonyl complexes, while no volataile complex of Hf and Ta were detected. This technique has been applied to a chemical investigation of the superheavy element Sg (atomic number 106), and will be applicable to various fields of nuclear science with short-lived transition metal isotopes.

Synthesis and detection of a Seaborgium carbonyl complex

Even, J.*; Yakushev, A.*; Dllmann, Ch. E.*; Haba, Hiromitsu*; Asai, Masato; Sato, Tetsuya; Brand, H.*; Di Nitto, A.*; Eichler, R.*; Fan, F. L.*; et al.

Science, 345(6203), p.1491 - 1493, 2014/09

https://doi.org/10.1126/science.1255720

A new superheavy element complex, a seaborgium carbonyl, has been successfully synthesized, and its adsorption property has been studied using a cryo-thermochromatography and -detection apparatus COMPACT. Nuclear reaction products of short-lived Sg preseparated with a gas-filled recoil ion separator GARIS at RIKEN were directly injected into a gas cell filled with He/CO mixture gas, and chemical reaction products of volatile carbonyl complexes were trasported to COMPACT. The Sg carbonyl complex detected with COMPACT was found to be very volatile with adsorption enthalpy of 50 kJ/mol, from which we have concluded that this complex should be a Sg hexacarbonyl Sg(CO). This is the first synthesis of organometallic compounds of transactinide elements for which only simple inorganic comounds have been synthesized so far.

Production of Db in the Cm(F,5)Db reaction and decay properties of Db and Lr

Haba, Hiromitsu*; Huang, M.*; Kaji, Daiya*; Kanaya, Jumpei*; Kudo, Yuki*; Morimoto, Koji*; Morita, Kosuke*; Murakami, Masashi*; Ozeki, Kazutaka*; Sakai, Ryutaro*; et al.

Physical Review C, 89(2), p.024618_1 - 024618_11, 2014/02

https://doi.org/10.1103/PhysRevC.89.024618

Isotope-selective ionization utilizing molecular alignment and non-resonant multiphoton ionization

Akagi, Hiroshi; Kasajima, Tatsuya; Kumada, Takayuki; Itakura, Ryuji; Yokoyama, Atsushi; Hasegawa, Hirokazu*; Oshima, Yasuhiro*

Applied Physics B, 109(1), p.75 - 80, 2012/10

https://doi.org/10.1007/s00340-012-5222-3

We demonstrate a laser nitrogen isotope separation, which is based on field-free alignment and angular dependent ionization of N and N isotopomers. A linearly-polarized short laser pulse (795 nm, 60 fs) creates rotational wave packets in the isotopomers, which periodically revive with different revival times as a result of different moments of inertia. Another linearly-polarized short laser pulse (795 nm, 60 fs) ionizes one of the isotopomers selectively as a result of their different angular distributions. In the present experiments, the ion yield ratio [= (N)/(N)] can be changed in the range from 0.85 to 1.22, depending on the time delay between the two laser pulses.