Initial oxidation processes of ultrathin hafnium film and hafnium disilicide islands on Si(100)-21 surfaces studied using core-level X-ray photoelectron spectroscopy

Kakiuchi, Takuhiro*; Yamasaki, Hideki*; Tsukada, Chie*; Yoshigoe, Akitaka

Surface Science, 693, p.121551_1 - 121551_8, 2020/03

https://doi.org/10.1016/j.susc.2019.121551

We investigated the initial oxidation of ultrathin hafnium (Hf) film on Si(100)-21 using photoelectron spectroscopy. Metallic Hf rapidly oxidized, transforming into hafnium dioxide (HfO) and its suboxides. The other HfSi component at the interface was nearly unreactive with O molecules. These facts suggest that the metallic Hf component plays a vital role in the initial oxidation of the ultrathin Hf/Si(100) film. After annealing from 873 K to 973 K, the Hf suboxides in low ionic valences progressed into fully oxidized HfO. Once the annealing temperature reached c.a.1073 K, oxygen atoms were entirely removed from the ultrathin HfO/Si(100) film containing SiO at the interface. Simultaneously, ultrathin HfO layers changed into islands of Hf disilicide (-HfSi) on a bare Si(100)-21 surface. The -HfSi component showed slight reactivity with O molecules at 298 K. In contrast to the initial oxidation of clean Si(100)-21 surface, the dangling bonds on bare Si(100)-21 surface among -HfSi oxidized preferentially.

Formation and thermochemical properties of oxychlorides of niobium (Nb) and tantalum (Ta); Towards the gas-phase investigation of dubnium (Db) oxychloride

Chiera, N. M.; Sato, Tetsuya; Tomitsuka, Tomohiro; Asai, Masato; Suzuki, Hayato*; Tokoi, Katsuyuki; Toyoshima, Atsushi; Tsukada, Kazuaki; Nagame, Yuichiro

Inorganica Chimica Acta, 486, p.361 - 366, 2019/02

https://doi.org/10.1016/j.ica.2018.10.032

The formation of NbOCl and TaOCl and their adsorption behavior on quartz surfaces was explored by applying an isothermal gas-chromatographic method. Trace amounts of short-lived Nb and Ta isotopes were used. Adsorption enthalpy values () at zero surface coverage of -(NbOCl) = 102 4 kJ/mol and -(TaOCl) = 128 5 kJ/mol were determined by analyzing the chromatographic behavior of the Nb andTa complexes with a Monte-Carlo simulation method based on an adsorption-desorption kinetic model.By applying an empirical correlation, the experimental values were successively related to the macroscopic standard sublimation enthalpy, , as a measure of the volatility of each substance. The inferred sublimation enthalpies are in agreement with tabulated thermochemical values. Thus, the linear empirical correlation between and for metal-oxychlorides was updated with the inclusion of the present data. According to the predicted (DbOCl), a (DbOCl) value of 135 2 kJ/mol was extrapolated. The future accomplishment of comparative studies with DbOCl under the same experimental conditions will provide valuable information on the volatility trend in Group-5 elements, together with an indication on the magnitude of relativistic effects on the electronic structure of dubnium.

Characterization of SiO reduction reaction region at void periphery on Si(110)

Yano, Masahiro; Uozumi, Yuki*; Yasuda, Satoshi; Tsukada, Chie*; Yoshida, Hikaru*; Yoshigoe, Akitaka; Asaoka, Hidehito

Japanese Journal of Applied Physics, 57(8S1), p.08NB13_1 - 08NB13_4, 2018/07

https://doi.org/10.7567/JJAP.57.08NB13

Initial oxidation of CuPd(111) surface

Tsuda, Yasutaka*; Makino, Takamasa*; Tsukada, Chie; Yoshigoe, Akitaka; Fukuyama, Tetsuya*; Okada, Michio*

no journal, , 

It is well-known that oxidation is an important chemical reactions in corrosion processes. CuPd has an attracting material due to its catalytic property and its oxidation is the important subject. In this presentation, initial oxidation processes at the CuPd(111) surface was studied by using molecular beams. In situ photoemission measurements were conducted using surface chemistry apparatus at BL23SU at SPring-8. Single crystal CuPd was used after cleaning by means of Ar ion sputtering and annealing. It was found that molecular beams facilitate oxidation compared to that for backfilling condition. Furthermore, diffusion of surface atoms seems to be driven with increasing surface temperature.

Reaction of CH on Cu(111) using supersonic CH molecular beam

Makino, Takamasa*; Tsuda, Yasutaka*; Tsukada, Chie; Yoshigoe, Akitaka; Okada, Michio*

no journal, , 

Studies on the interaction between ethylene molecule and metal surfaces are the important subject to understand catalyitic reactions such as dehydrogenation. To clarify dissociation adsorption processes of ethylene at metal surfaces, the surface analysis after exposure of ethylene to Cu(111) surface was conducted by using synchrotron radiation XPS. We found the growth of peak intensities and the peak shifted to higher binding energy side when ethylene beams with the kinetic energy of 2 eV were irradiated at the surface temperature of 300 K. The adsorption states and surface temperature dependece of reactions will be discussed.

Development of low energy atomic beam extraction technique for determination of valence electronic structure of Lawrencium (Z = 103)

Tomitsuka, Tomohiro; Tokoi, Katsuyuki*; Sato, Tetsuya; Asai, Masato; Tsukada, Kazuaki; Toyoshima, Atsushi; Chiera, N. M.; Kamada, Hiroki; Nagame, Yuichiro; Goto, Shinichi*

no journal, , 

no abstracts in English

Spontaneous fission measurements for nuclei around neutron-rich Fm region produced by using an Es target

Asai, Masato; Tsukada, Kazuaki; Hirose, Kentaro; Toyoshima, Atsushi; Tomitsuka, Tomohiro; Chiera, N. M.; Ito, Yuta; Makii, Hiroyuki; Nagame, Yuichiro; Nishio, Katsuhisa; et al.

no journal, , 

Spontaneous fissions of Fm, Fm, and Lr have been measured using an Es target at the JAEA Tandem Accelerator Facility. These three nuclei show different fission properties: the asymmetric fission, the high total-kinetic-energy (TKE) symmetric fission, and the low TKE symmetric fission, and the mechanisms of these three fissions should be very different. It is of great interest to elucidate how these differences occur. We have produced Fm in multinucleon-transfer reactions with a Es target and O projectiles, and produced Lr in the Cm(N,4n) fusion-evaporation reaction. The reaction products were mass-separated with a gas-jet-coupled on-line isotope separator, and were delivered into a rotating wheel alpha- and fission-fragment detection system. By comparing the mass and TKE distributions deduced from the present experimental data, we will discuss the differences in fission mechanism among Fm, Fm, and Lr.

Spontaneous fission measurements for neutron-rich Fm and Lr isotopes using Es target

Asai, Masato; Tsukada, Kazuaki; Hirose, Kentaro; Toyoshima, Atsushi*; Tomitsuka, Tomohiro*; Chiera, N. M.*; Ito, Yuta; Makii, Hiroyuki; Nagame, Yuichiro*; Nishio, Katsuhisa; et al.

no journal, , 

Neutron-rich fermium isotopes Fm and Fm and lawrencium isotope Lr were produced in the multinucleon transfer reaction on Es target with heavy-ion beam and in the heavy-ion fusion reaction on Cm target with N beam, respectively. Reaction products were mass-separated with an on-line isotope separator (ISOL), and spontaneous fission (SF) of these isotopes were measured. It was found that the mass distribution of the SF of Fm was asymmetric, while that of Fm was sharp symmetric, which confirmed the previous experimental results. On the other hand, the SF of Lr seemed to contain both symmetric and asymmetric mass distributions. On the basis of the present results of the mass and total kinetic energy distributions, we discussed the mechanism of fission for these isotopes.

Spontaneous fission studies for neutron-rich Fm and Lr isotopes

Asai, Masato; Tsukada, Kazuaki; Hirose, Kentaro; Toyoshima, Atsushi*; Tomitsuka, Tomohiro*; Chiera, N. M.*; Ito, Yuta; Makii, Hiroyuki; Nagame, Yuichiro*; Nishio, Katsuhisa; et al.

no journal, , 

We have studied spontaneous fission of neutron-rich Fm and Lr isotopes. The neutron-rich Fm isotopes were produced with the Es target and the O beam delivered by the JAEA tandem accelerator. The neutron-rich Lr isotope were produced with the Cm target and the N beam. Reaction products were mass-separated with an on-line isotope separator (ISOL), which enabled us to obtain non-contaminated samples and to measure fission fragments precisely. From the deduced fission-fragment mass and total kinetic energy distributions, we have obtained a new insight into the competition between the symmetric and asymmetric fission which is characteristic in this neutron-rich region.

Fission of Md produced in the He + Es reaction

Nishio, Katsuhisa; Hirose, Kentaro; Makii, Hiroyuki; Orlandi, R.; Kean, K. R.*; Tsukada, Kazuaki; Toyoshima, Atsushi*; Asai, Masato; Sato, Tetsuya; Chiera, N. M.*; et al.

no journal, , 

no abstracts in English