Detecting halfmetallic electronic structures of spintronic materials in a magnetic field

Fujiwara, Hidenori*; Umetsu, Rie*; Kuroda, Fumiaki*; Miyawaki, Jun*; Kashiuchi, Toshiyuki*; Nishimoto, Kohei*; Nagai, Kodai*; Sekiyama, Akira*; Irizawa, Akinori*; Takeda, Yukiharu; et al.

Scientific Reports (Internet), 11(1), p.18654_1 - 18654_9, 2021/09

https://doi.org/10.1038/s41598-021-97992-z

Electronic structure and magnetic properties of the half-metallic ferrimagnet MnVAl probed by soft X-ray spectroscopies

Nagai, Kodai*; Fujiwara, Hidenori*; Aratani, Hidekazu*; Fujioka, Shuhei*; Yomosa, Hiroshi*; Nakatani, Yasuhiro*; Kiss, Takayuki*; Sekiyama, Akira*; Kuroda, Fumiaki*; Fujii, Hitoshi*; et al.

Physical Review B, 97(3), p.035143_1 - 035143_8, 2018/01

AA2017-0644.pdf:1.01MB

https://doi.org/10.1103/PhysRevB.97.035143

We have studied the electronic structure of ferrimagnetic MnVAl single crystals by means of soft X-ray absorption spectroscopy (XAS), X-ray absorption magnetic circular dichroism (XMCD), and resonant soft X-ray inelastic scattering (RIXS). We have successfully observed the XMCD signals for all the constituent elements. The Mn L XAS and XMCD spectra are reproduced by spectral simulations based on density-functional theory, indicating the itinerant character of the Mn 3 states. On the other hand, the V 3 electrons are rather localized since the ionic model can qualitatively explain the V L XAS and XMCD spectra. This picture is consistent with local excitations revealed by the V L RIXS.

Observation of momentum-dependent charge excitations in hole-doped cuprates using resonant inelastic X-ray scattering at the oxygen edge

Ishii, Kenji*; Toyama, Takami*; Asano, Shun*; Sato, Kentaro*; Fujita, Masaki*; Wakimoto, Shuichi; Tsutsui, Kenji*; Sota, Shigetoshi*; Miyawaki, Jun*; Niwa, Hideharu*; et al.

Physical Review B, 96(11), p.115148_1 - 115148_8, 2017/09

AA2017-0402.pdf:0.81MB

https://doi.org/10.1103/PhysRevB.96.115148

Electronic structure of Pt and Pt-Co nanoparticles with O and O/HO adsorption revealed by in situ XAFS and hard X-ray photoelectron spectroscopy

Cui, Y.*; Harada, Yoshihisa*; Hatanaka, Tatsuya*; Nakamura, Naoki*; Ando, Masaki*; Yoshida, Toshihiko*; Ikenaga, Eiji*; Ishii, Kenji*; Matsumura, Daiju; Li, R.*; et al.

ECS Transactions, 72(8), p.131 - 136, 2016/10

https://doi.org/10.1149/07208.0131ecst

Precise determination of precipitation yield of uranyl nitrate with -alkylated 2-pyrrolidone derivatives

Takao, Koichiro*; Kawata, Yoshihisa*; Nogami, Masanobu*; Harada, Masayuki*; Morita, Yasuji; Nishimura, Kenji*; Ikeda, Yasuhisa*

Journal of Nuclear Science and Technology, 52(2), p.294 - 298, 2015/02

https://doi.org/10.1080/00223131.2014.937782

Yields of precipitated UO(NO)(NRP) (NRP = -alkylated 2-pyrrolidone) were precisely determined by considering reduction of the solution volume through the precipitation, which can be estimated from difference in acid concentrations of the liquid phases before and after the precipitation. The studied NRPs were --butyl (NBP) and --propyl (NProP) derivatives. In both systems, the precipitation yields precisely determined were always higher than those simply calculated from the ratio of uranium concentrations before and after the precipitation. However, the differences between them are in the range of 0.6% - 2.6%. If such a difference is practically negligible, the volume reduction through the precipitation does not have to be taken into account for simplicity of the analytical manipulation.

Unveiling the impurity band induced ferromagnetism in the magnetic semiconductor (Ga,Mn)As

Kobayashi, Masaki*; Muneta, Iriya*; Takeda, Yukiharu; Harada, Yoshihisa*; Fujimori, Atsushi*; Krempask, J.*; Schmitt, T.*; Oya, Shinobu*; Tanaka, Masaaki*; Oshima, Masaharu*; et al.

Physical Review B, 89(20), p.205204_1 - 205204_8, 2014/05

https://doi.org/10.1103/PhysRevB.89.205204

Probing carbon edge exposure of iron phthalocyanine-based oxygen reduction catalysts by soft X-ray absorption spectroscopy

Niwa, Hideharu*; Saito, Makoto*; Kobayashi, Masaki*; Harada, Yoshihisa*; Oshima, Masaharu*; Moriya, Shogo*; Matsubayashi, Katsuyuki*; Nabae, Yuta*; Kuroki, Shigeki*; Ikeda, Takashi; et al.

Journal of Power Sources, 223, p.30 - 35, 2013/02

https://doi.org/10.1016/j.jpowsour.2012.09.031

To design non-platinum, inexpensive, but high performance carbon-based cathode catalysts for polymer electrolyte fuel cells, it is important to elucidate the active site for oxygen reduction reaction (ORR). However, it is difficult to directly identify the active site by applying conventional structural or electronic probes to such complex systems. Here, we used C 1 X-ray absorption spectroscopy (XAS) to observe electronic structure of carbon in iron phthalocyanine-based catalysts, and found a signature of edge exposure below the edge, whose intensity is well correlated with the ORR activity. These results demonstrate that C 1 XAS can be used to characterize the ORR activity of carbon-based cathode catalysts in terms of the edge exposure.

Stability of pyrrolidone derivatives against -ray irradiation

Nogami, Masanobu*; Sugiyama, Yuichi*; Kawasaki, Takeshi*; Harada, Masayuki*; Kawata, Yoshihisa*; Morita, Yasuji; Kikuchi, Toshiaki*; Ikeda, Yasuhisa*

Science China; Chemistry, 55(9), p.1739 - 1745, 2012/09

https://doi.org/10.1007/s11426-012-4698-3

Stability of N-alkylated pyrrolidone derivatives (NRPs) against radiation was examined by irradiation tests with Co -ray. We have been developed a novel reprocessing system using NRPs which have precipitation ability to haxa- and tetravalent actinides in nitric acid media. Degradation rates of NRPs are evaluated by irradiation in 3M nitric acid solutions and mechanism of degradation are discussed in the present paper.

Indirect contribution of transition metal towards oxygen reduction reaction activity in iron phthalocyanine-based carbon catalysts for polymer electrolyte fuel cells

Kobayashi, Masaki*; Niwa, Hideharu*; Saito, Makoto*; Harada, Yoshihisa*; Oshima, Masaharu*; Ofuchi, Hironori*; Terakura, Kiyoyuki*; Ikeda, Takashi; Koshigoe, Yuka*; Ozaki, Junichi*; et al.

Electrochimica Acta, 74, p.254 - 259, 2012/07

https://doi.org/10.1016/j.electacta.2012.04.075

The electronic structure of the residual metal atoms in FePc-based carbon catalysts, prepared by pyrolyzing a mixture of FePc and phenolic resin polymer at 800C, before and after acid washing have been investigated using XAFS spectroscopy to clarify the role of Fe in the ORR activity. The decomposition analyses for the XAFS spectra reveal that the composition ratio of each Fe component is unaltered by the acid washing, indicating that the residual Fe components were removed by the acid washing irrespective of their chemical states. Because the oxygen reduction potential was approximately unchanged by the acid washing, the residual Fe itself does not seem to contribute directly to the ORR activity. The residual Fe can act as a catalyst to accelerate the growth of the sp carbon network during pyrolysis. The results imply that light elements are components of the ORR active sites in the FePc-based carbon catalysts.

Role of residual transition-metal atoms in oxygen reduction reaction in cobalt phthalocyanine-based carbon cathode catalysts for polymer electrolyte fuel cell

Kobayashi, Masaki*; Niwa, Hideharu*; Harada, Yoshihisa*; Horiba, Koji*; Oshima, Masaharu*; Ofuchi, Hironori*; Terakura, Kiyoyuki*; Ikeda, Takashi; Koshigoe, Yuka*; Ozaki, Junichi*; et al.

Journal of Power Sources, 196(20), p.8346 - 8351, 2011/10

https://doi.org/10.1016/j.jpowsour.2011.06.062

The electronic structure of Co atoms in CoPc-based carbon catalysts, which were prepared by pyrolyzing a mixture of CoPc and phenol resin polymer up to 1000C, has been investigated using XAFS analysis and HXPES. The Co K XAFS spectra show that most of the Co atoms are in the metallic state and small quantities of oxidized Co components are present in the samples even after acid washing to remove Co atoms. Based on the difference in probing depth between XAFS and HXPES, it was found that after acid washing, the surface region with the aggregated Co clusters is primarily composed of metallic Co. Since the electrochemical properties remain almost unchanged even after the acid washing process, the residual metallic and oxidized Co atoms themselves will hardly contribute to the ORR activity of the CoPc-based carbon cathode catalysts, implying that the active sites of the CoPc-based catalysts primarily consist of light elements such as C and N.