論文 - 石丸　学

スパッタリング法によるアモルファスFe-B合金薄膜の作製と透過型電子顕微鏡による構造解析 査読有り

仲村 龍介, 半谷 祐樹, 石丸 学, 和田 武

鉄と鋼 ( 日本鉄鋼協会 )   105 ( 10 )   1017 - 1021   2019年01月

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記述言語：日本語   掲載種別：研究論文（学術雑誌）

<p>Amorphous Fe-B thin films of the concentration range between 12 and 25 at.% B were prepared by radio frequency sputtering techniques, and their local structures were examined by transmission electron microscopy. Pair-distribution-function analyses of Fe-12, -18 and -25 at.%B for a region of 300 nm in diameter revealed a systematic trend according to the concentration; with the increase in B concentration, the intensity of the weak shoulder peak at 0.205 nm for the Fe-B pair increases whereas those of main peaks for Fe-Fe pair decrease. In electron diffraction patterns of the samples taken by a probe size of 2 nm, the specific spots of iron-borides, such as Fe₃B and Fe₂₃B₆, were detected, suggesting the atomic arrangement of the compounds in the amorphous matrices.</p>

DOI： 10.2355/tetsutohagane.TETSU-2019-032

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Deposition-temperature dependence of vortex pinning property in YBa<inf>2</inf>Cu<inf>3</inf>O<inf>7</inf>+BaHfO<inf>3</inf> Film 査読有り

Horide T., Torigoe K., Kita R., Nakamura R., Ishimaru M., Awaji S., Matsumoto K.

Nippon Kinzoku Gakkaishi/Journal of the Japan Institute of Metals ( 公益社団法人 日本金属学会 )   83 ( 9 )   320 - 326   2019年01月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2019 The Japan Institute of Metals and Materials. Improvement of critical current density (Jc) in magnetic fields is required in YBa2Cu3O7 films, and process parameters should be optimized for controlling pinning centers. In the present study, a deposition temperature was varied in pulsed laser deposition of YBa2Cu3O7+BaHfO3 films to control the nanorod structure, and its influence on Jc was analyzed. The YBa2Cu3O7+BaHfO3 film deposited at 850°C exhibited pinning force maximum(Fp,max) as high as 413 GN/m3 at 40 K, while the Fp,max for the deposition temperature of 850°C at 77 K was smaller than that in the YBa2Cu3O7+BaHfO3 film deposited at 900°C. A critical temperature decreased and matching field increased with decreasing the deposition temperature. Increase in deposition temperature is effective in improving the Fp,max in high temperatures, since the critical temperature and matching field dependences of Jc value dominate the Fp,max. On the other hand, low deposition temperature improves the Fp,max in low temperatures since the Fp shift in accordance with matching field is dominant to the Fp,max. Thus, the deposition temperature should be set in pulsed laser deposition of YBa2Cu3O7 films containing nanorods considering the Jc variation with critical temperature and matching field.

DOI： 10.2320/jinstmet.JA201902

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Application of the Tersoff interatomic potential to pressure-induced polyamorphism of silicon 査読有り 国際誌

Mukuno R., Ishimaru M.

Japanese Journal of Applied Physics   58 ( 10 )   2019年01月

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担当区分：責任著者   記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2019 The Japan Society of Applied Physics. Molecular-dynamics simulations of the pressure-induced structural changes of amorphous Si have been performed using the Tersoff interatomic potential to examine the validity of this potential. Amorphous Si with a tetrahedral network was prepared by melt-quenching methods, and it was then compressed under isothermal-isobaric conditions. The changes of the atomic pair-distribution functions and static structure factors with increasing pressure were in agreement with those observed experimentally. The pressure-induced amorphous structures contained a short-range order similar to the β-tin and Imma structures. These results suggest that the Tersoff potential is suitable for describing the structural changes of amorphous Si under high pressure.

DOI： 10.7567/1347-4065/ab42f3

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Chalcopyrite ZnSnSb<inf>2</inf>: A Promising Thermoelectric Material 査読有り

Nomura A., Choi S., Ishimaru M., Kosuga A., Chasapis T., Ohno S., Snyder G., Ohishi Y., Muta H., Yamanaka S., Kurosaki K.

ACS Applied Materials and Interfaces   10 ( 50 )   43682 - 43690   2018年12月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2018 American Chemical Society. Ternary compounds with a tetragonal chalcopyrite structure, such as CuGaTe2, are promising thermoelectric (TE) materials. It has been demonstrated in various chalcopyrite systems, including compounds with quaternary chalcopyrite-like structures, that the lattice parameter ratio, c/a, being exactly 2.00 to have a pseudo-cubic structure is key to increase the degeneracy at the valence band edge and ultimately achieve high TE performance. Considering the fact that ZnSnSb2 with a chalcopyrite structure is reported to have c/a close to 2.00, it is expected to have multiple valence bands leading to a high p-type zT. However, there are no complete investigations on the high temperature TE properties of ZnSnSb2 mainly because of the difficulty of obtaining a single-phase ZnSnSb2. In the present study, pure ZnSnSb2 samples with no impurities are synthesized successfully using a Sn flux-based method and TE properties are characterized up to 585 K. Transport properties and thermal analysis indicate that the structure of ZnSnSb2 remains chalcopyrite with no order-disorder transition and clearly show that ZnSnSb2 can be made to exhibit a high zT in the low-to-mid temperature range through further optimization.

DOI： 10.1021/acsami.8b16717

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Structure of crystallized particles in sputterdeposited amorphous germanium films 査読有り

Okugawa M., Nakamura R., Hirata A., Ishimaru M., Yasuda H., Numakura H.

Journal of Applied Crystallography   51 ( 5 )   1467 - 1473   2018年10月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2018 International Union of Crystallography. Pristine thin films of amorphous Ge prepared by sputtering are unstable and form coarse crystalline particles of 100 nm in size upon crystallization by electron irradiation. These crystalline particles exhibit unusual diffraction patterns that cannot be understood from the diamond cubic structure. The structure has previously been assumed to be a metastable hexagonal form. In the present work, the structure of the coarse crystalline particles has been analysed in detail by transmission electron microscopy, considering the possibility that those diffraction patterns might occur with the diamond cubic structure if the particle consists of thin twin layers. By high-resolution lattice imaging the particles have been shown to be of the diamond cubic structure containing a high density of twins and stacking faults parallel to {111}. With such defects, diffraction patterns can be complex because of the following effects: superposition of two or more diffraction patterns of the same structure but of different orientations, double diffraction through twin crystals, and streaks parallel to the thin crystal which give rise to extra diffraction spots. It is found that diffraction patterns taken from various orientations can be explained in terms of these effects.

DOI： 10.1107/S1600576718012153

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Molecular-dynamics simulations of solid phase epitaxy in silicon: Effects of system size, simulation time, and ensemble 査読有り

Kohno K., Ishimaru M.

Japanese Journal of Applied Physics   57 ( 9 )   2018年09月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2018 The Japan Society of Applied Physics. Solid phase epitaxial (SPE) recrystallization of amorphous Si on a Si(001) substrate was examined by large-scale (6144-129024 Si atoms), longtime (up to 2000 ns) molecular-dynamics (MD) simulations using the empirical Tersoff interatomic potential. We particularly focused on the effects of the MD cell size, simulation time, and ensemble on the SPE growth rate. We found that the simulations under the isothermal-isochoric conditions (NVT ensemble) show a higher crystallization rate than those under the isothermal-isobaric conditions (NPT ensemble). The system size dealt with in the present MD simulation, i.e., >6144 Si atoms, was enough to estimate the SPE growth rate. The Arrhenius plot of the growth rate between 1300 and 1600 K exhibited a single activation energy, >2.4 eV, which is in agreement with the experimental value (>2.7 eV). However, the growth rate at temperatures below 1300 K deviated from the extrapolated ones from 1300 to 1600 K, which is because recrystallization does not reach a steady state: long-time MD simulations are required to estimate the growth rate at low temperature. The structure analysis of amorphous/ crystalline interfaces suggested that the braking of atomic bonds parallel to the interface becomes a rate-limiting step of the SPE growth.

DOI： 10.7567/JJAP.57.095503

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Geometric and compositional factors on critical current density in YBa<inf>2</inf>Cu<inf>3</inf>O<inf>7-δ</inf>films containing nanorods 査読有り

Horide T., Nagao S., Izutsu R., Ishimaru M., Kita R., Matsumoto K.

Superconductor Science and Technology   31 ( 6 )   2018年05月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2018 IOP Publishing Ltd. Critical current density (Jc) was investigated in YBa2Cu3O7-δfilms containing nanorods prepared with various nanorod materials, with variation of nanorod content, substrate temperature, and oxidization condition. Three types of compositional situation were realized: films containing strain induced oxygen vacancies; fully oxidized films containing cation compositional deviation; and oxygen deficient films. Normalized Jc-B behavior was determined via the matching field, which is a geometric factor, regardless of the compositional details. A Jc-critical temperature (Tc) relation depending on distribution and fraction of compositional deviation (cation compositional deviation and strain induced oxygen vacancies) was found: the Jcvalues decreased with decreasing Tcdue to the effect of Tcon nanorod pinning strength in the fully oxidized films; Jcdecreased with decreasing oxygen pressure in the film cooling process after film deposition in spite of Tcremaining almost the same, due to reduction of the effective area for current flow in the oxygen deficient films. Thus, a Jclandscape based on geometric and compositional factors was obtained. The study highlights the importance of the Jc-Tcanalysis in the understanding of Jcin YBa2Cu3O7-δfilms containing nanorods.

DOI： 10.1088/1361-6668/aabe68

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第12回ミクロ・ナノ解析に関する日本・ポーランド合同セミナー開催報告 査読有り

石丸 学

まてりあ ( 公益社団法人 日本金属学会 )   57 ( 12 )   631 - 631   2018年01月

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担当区分：筆頭著者   記述言語：日本語   掲載種別：記事・総説・解説・論説等（学術雑誌）

DOI： 10.2320/materia.57.631

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Proton-Driven Intercalation and Ion Substitution Utilizing Solid-State Electrochemical Reaction 査読有り

Fujioka M., Wu C., Kubo N., Zhao G., Inoishi A., Okada S., Demura S., Sakata H., Ishimaru M., Kaiju H., Nishii J.

Journal of the American Chemical Society   139 ( 49 )   17987 - 17993   2017年12月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2017 American Chemical Society. The development of an unconventional synthesis method has a large potential to drastically advance materials science. In this research, a new synthesis method based on a solid-state electrochemical reaction was demonstrated, which can be made available for intercalation and ion substitution. It was referred to as proton-driven ion introduction (PDII). The protons generated by the electrolytic dissociation of hydrogen drive other monovalent cations along a high electric field in the solid state. Utilizing this mechanism, Li + , Na + , K + , Cu + , and Ag + were intercalated into a layered TaS 2 single crystal while maintaining high crystallinity. This liquid-free process of ion introduction allows the application of high voltage around several kilovolts to the sample. Such a high electric field strongly accelerates ion substitution. Actually, compared to conventional solid-state reaction, PDII introduced 15 times the amount of K into Na super ionic conductor (NASICON)-structured Na 3-x K x V 2 (PO 4 ) 3 . The obtained materials exhibited a thermodynamically metastable phase, which has not been reported so far. This concept and idea for ion introduction is expected to form new functional compounds and/or phases.

DOI： 10.1021/jacs.7b09328

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Helium Irradiation and Implantation Effects on the Structure of Amorphous Silicon Oxycarbide 査読有り

Su Q., Inoue S., Ishimaru M., Gigax J., Wang T., Ding H., Demkowicz M., Shao L., Nastasi M.

Scientific Reports   7 ( 1 )   2017年12月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2017 The Author(s). Despite recent interest in amorphous ceramics for a variety of nuclear applications, many details of their structure before and after irradiation/implantation remain unknown. Here we investigated the short-range order of amorphous silicon oxycarbide (SiOC) alloys by using the atomic pair-distribution function (PDF) obtained from electron diffraction. The PDF results show that the structure of SiOC alloys are nearly unchanged after both irradiation up to 30 dpa and He implantation up to 113 at%. TEM characterization shows no sign of crystallization, He bubble or void formation, or segregation in all irradiated samples. Irradiation results in a decreased number of Si-O bonds and an increased number of Si-C and C-O bonds. This study sheds light on the design of radiation-tolerant materials that do not experience helium swelling for advanced nuclear reactor applications.

DOI： 10.1038/s41598-017-04247-x

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Formation of metastable phases in Zr-ion-irradiated Al<inf>2</inf>O<inf>3</inf>upon thermal annealing 査読有り

Oka N., Ishimaru M., Tane M., Sina Y., McHargue C., Sickafus K., Alves E.

Microscopy   66 ( 6 )   388 - 396   2017年12月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© The Author 2017. Published by Oxford University Press on behalf of The Japanese Society of Microscopy. All rights reserved. Formation of metastable phases in Zr-ion-irradiated corundum alumina (Al 2 O 3 ) upon thermal annealing was examined using transmission electron microscopy. A metastable cubic spinel phase was formed in the topmost layer of the as-irradiated microstructure. During thermal annealing at temperatures ranging from 1073 to 1273 K, this spinel layer grew in extent via an unusual corundum-to-spinel phase transformation. A normal spinel-to-corundum phase transformation was observed at post-irradiation annealing temperatures greater than 1473 K. In addition, ZrO 2 nanocrystals embedded in α-Al 2 O 3 were observed to form at these higher temperatures. High-resolution transmission electron microscopy observations and electron diffraction experiments revealed that the structure of the ZrO 2 precipitates observed in this study are consistent with a highpressure metastable orthorhombic phase of ZrO 2 known as the Ortho-I phase.

DOI： 10.1093/jmicro/dfx028

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Low-temperature synthesis of crystalline GeSn with high Sn concentration by electron excitation effect 査読有り

Kimura T., Ishimaru M., Okugawa M., Nakamura R., Yasuda H.

Japanese Journal of Applied Physics   56 ( 10 )   2017年10月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2017 The Japan Society of Applied Physics. The low-temperature synthesis of high-Sn-concentration GeSn is challenging in realizing flexible thin-film transistors and solar cells. Because of athermal processes, irradiation with energetic particles is anticipated to significantly reduce the processing temperature for device fabrication. Here, we demonstrated that polycrystalline Ge with 30 at.% Sn can be realized at room temperature by the electron-beam-induced recrystallization of amorphous GeSn. We found that inelastic electronic stopping, the so-called electron excitation effect, plays an important role in the recrystallization of amorphous GeSn.

DOI： 10.7567/JJAP.56.100307

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Inhomogeneous crystallization of sputter-deposited amorphous Ge films 査読有り

Nakamura R., Okugawa M., Ishimaru M., Yasuda H., Numakura H.

AM-FPD 2017 - 24th International Workshop on Active-Matrix Flatpanel Displays and Devices: TFT Technologies and FPD Materials, Proceedings   276 - 278   2017年08月

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記述言語：英語   掲載種別：研究論文（国際会議プロシーディングス）

Crystallization of amorphous germanium films induced by electron irradiation was investigated by in-situ transmission electron microscopy under a low electron-eneigy of 125 keV with various pre-Aging treatments at room temperature. Different microstructures were observed depending on the aging time: coarse and spherical nanoparticles grew rapidly in samples aged for less than 3 months, while a homogeneous nanociystalline structure with a grain size of about 10 nm appealed in samples aged for over 7 months. Analyses by the pair distribution lunction revealed that the initial structure is inhomogeneous, consisting of a mixture of amorphous regions and some ordered arrangements, but turned spontaneously to homogeneous random amorphous structures during aging. Such inhomogeneity could be an origin of the rapid growth of nanoparticles in the samples not subjected to the long-Time aging.

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Strong c-axis correlated pinning and hybrid pinning in YBa<inf>2</inf>Cu<inf>3</inf>O<inf>7-δ</inf> films containing BaHfO<inf>3</inf> nanorods and stacking faults 査読有り

Horide T., Otsubo K., Kita R., Matsukida N., Ishimaru M., Awaji S., Matsumoto K.

Superconductor Science and Technology   30 ( 7 )   2017年06月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2017 IOP Publishing Ltd. High critical current density (J c ) was achieved in low temperatures of 40 and 20 K in YBa 2 Cu 3 O 7-δ films containing elongated BaHfO 3 nanorods and stacking faults, which were prepared using pulsed laser deposition and post-oxygen-annealing. The YBa 2 Cu 3 O 7-δ + BaHfO 3 film exhibited global pinning force maximum (F p,max ) of 312 GNm -3 at 40 K and 619 GNm -3 at 20 K due to strong pinning by nanorods. These Fp,max values are comparable to those in the previously-reported high-J c films with almost the same matching field. Thus, the present study demonstrated that YBa 2 Cu 3 O 7-δ superconducting matrix realized high J c in low temperatures like other REBa 2 Cu 3 O 7-δ (RE = Gd, Sm, (Gd, Y)). Furthermore, high J c was obtained also for magnetic field parallel to the ab-plane, indicating hybrid pinning of nanorods and stacking faults. Thus, the stacking faults significantly affected the J c properties in the YBa 2 Cu 3 O 7-δ films containing nanorods.The present film structure with strong c-axis correlated pinning and hybrid pinning is effective in simultaneous control of J c values and J c anisotropy in YBa 2 Cu 3 O 7-δ films.

DOI： 10.1088/1361-6668/aa70d3

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Pin potential effect on vortex pinning in YBa<inf>2</inf>Cu<inf>3</inf>O<inf>7-δ</inf> films containing nanorods: Pin size effect and mixed pinning 査読有り

Horide T., Matsukida N., Ishimaru M., Kita R., Awaji S., Matsumoto K.

Applied Physics Letters   110 ( 5 )   2017年01月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2017 Author(s).The pin size effect and mixed pinning of nanorods and matrix defects are discussed for YBa2Cu3O7-δ films containing nanorods. BaSnO3 nanorods with a diameter of 11 nm and BaHfO3 nanorods with a diameter of 7 nm were prepared, and critical current density (Jc) and resistivity were measured in the films. When the coherence length was larger than the nanorod size at high temperatures near the critical temperature, the trapping angle and activation energy of the vortex flow depended on the nanorod diameter. At a moderate temperature of 65−77 K, the pin size effect on Jc disappeared since the coherence length became smaller than the nanorod size. At a low temperature of 20 K, the contribution from matrix pinning became comparable to that of nanorods in a high magnetic field due to the small coherence length. Thus, the temperature-dependent coherence length caused the pin potential situation to vary significantly, namely, the pin size effect and mixed pinning, which strongly affected vortex pinning in YBa2Cu3O7-δ containing nanorods.

DOI： 10.1063/1.4975300

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Molecular dynamics study on structural relaxation processes in amorphous germanium 査読有り

Imabayashi S., Ishimaru M.

Materials Transactions   58 ( 6 )   857 - 861   2017年01月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

© 2017 The Japan Institute of Metals and Materials.The structural relaxation of amorphous germanium was examined by molecular dynamics simulations based on the empirical Tersoff interatomic potential. Although the Tersoff potential overestimated both the melting and glass transition temperatures, it was able to reproduce the structural relaxation behavior. The potential energy decreases with thermal annealing below the glass transition temperature, but occasionally increases during structural relaxation. The mean square displacement of atoms also increases in these periods. These changes were attributed to cooperative atomic motion during the structural relaxation. Atomic trajectories revealed that structural changes are induced by spatially- and temporally-inhomogeneous atomic motions: atomically mobile and immobile regions coexist during structural relaxation.

DOI： 10.2320/matertrans.M2017036

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アモルファスGeにおける構造緩和過程の分子動力学法による解析 査読有り

Imabayashi S., Ishimaru M.

日本金属学会誌   81 ( 2 )   66 - 70   2017年01月

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記述言語：日本語   掲載種別：研究論文（学術雑誌）

© 2016 The Japan Institute of Metals and Materials.Structural relaxation of amorphous germanium has been examined by molecular dynamics simulations based on the empirical Tersoff interatomic potential. Although the Tersoff potential overestimated both the melting and glass transition temperatures, it was found that this potential can reproduce the behavior of structural relaxation. The potential energy decreased with thermal annealing below the glass transition temperature, but it sometimes increased during structural relaxation. The mean square displacement of atoms also increased at the corresponding period. These changes were attributed to the cooperative atomic motion during structure relaxation. Atomic trajectories revealed that structural changes are induced by spatially- and temporally-inhomogeneous atomic motions: atomic mobile and immobile regions coexisted during structural relaxation.

DOI： 10.2320/jinstmet.J2016051

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透過電子顕微鏡法による照射誘起構造変化の解析 招待有り 査読有り

石丸 学

顕微鏡 ( 公益社団法人 日本顕微鏡学会 )   52 ( 1 )   24 - 28   2017年01月

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担当区分：筆頭著者   記述言語：日本語   掲載種別：記事・総説・解説・論説等（学術雑誌）

<p>照射場を利用した材料創製では，通常の手法では得ることが難しい平衡状態から離れた準安定構造を実現することが出来る．また，機能性材料および構造用材料の照射誘起構造変化に関する研究は，宇宙空間や原子炉等の極限環境下で使用される材料の信頼性を知る上で重要である．本稿では，照射場と材料の相互作用による構造変化およびそれを利用した材料創製に関する最近の研究成果について報告する．準安定構造の形成に関しては，イオン照射アルミナの熱処理過程において見出された，通常の熱処理では起こらないコランダム→スピネル型構造相変態について報告する．一方，耐照射性材料の開発に関する一連の研究では，ナノ構造制御により炭化ケイ素の耐照射性を向上させた例について紹介する．</p>

DOI： 10.11410/kenbikyo.52.1_24

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Behavior of Sn atoms in GeSn thin films during thermal annealing: Ex-situ and in-situ observations 査読有り

R. Takase, M. Ishimaru, N. Uchida, T. Maeda, K. Sato, R. R. Lieten, J.-P. Locquet

Journal of Applied Physics   120   245304(1) - 245304(9)   2016年12月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

DOI： 10.1063/1.4973121

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Thermal crystallization of sputter-deposited amorphous Ge films: Competition of diamond cubic and hexagonal phases 査読有り

M. Okugawa, R. Nakamura, M. Ishimaru, H. Yasuda, H. Numakura

AIP Advances   6   125035(1) - 125035(9)   2016年12月

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記述言語：英語   掲載種別：研究論文（学術雑誌）

DOI： 10.1063/1.4972282

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