1.(1)-3) J. Am. Chem. Soc., 129, 3084 (2007). 物性化学研究室 研究ハイライト (1) イプシロン型 ガリウム酸化鉄からなるミリ波吸吸体イプシロン型 酸化鉄という特殊なナノ磁性体の鉄イオンの一部をガリウムイオンで置換した イプシロン型 ガリウム酸化鉄 (
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1 SOLID STATE PHYSICAL CHEMISTRY Annual Research Highlights (1) Millimeter Wave Absorption Millimeter waves are beginning to be used in electronic devices for high-speed wireless communication. However, materials that effectively restrain electromagnetic interference (EMI) in the region of millimeter waves almost do not exist. This time Prof. Shin-ichi Ohkoshi (Department of Chemistry, School of Science, The University of Tokyo) et al., developed a new EM absorber composed of ε-fe 2 O 3 (0.10 x 0.67) nanomagnets, which shows a ferromagnetic resonance in the region of GHz. In addition, the possibility that the resonance frequency can achieve 200GHz at x 0 is also suggested. The millimeter wave absorber of f r > 80GHz based on a magnetic material has not been reported to date. The present developed materials are suitable for an absorber to restrain the EMI (for example, a millimeter wave absorber painted on the wall of office, private and medical room, or the body of car, train, and airplane), and an optoelectronic device to stabilize the EM sending (for example, a circulator and an isolator for millimeter waves of needless magnetic field). Furthermore, because our materials are composed of a metal oxide, it is stable over long periods, and such millimeter wave absorbers are advantageous for industrial applications. due to the mixing of Fe vacancies and Fe II, Fe III, Mn II, and Jahn-Teller-distorted Mn III centers, and the ferromagnetism is mainly caused by a parallel Fig. 2 the coexistence of ferroelectricity and ferromagnetism in Rb 0.82 Mn[Fe(CN) 6 ] 0.94 H 2 O ordering of the magnetic spins on the Mn III centers. 1.(1)-2) Angew. Chem. Int. Ed., 46, 3238 (2007). (highlighted in the frontispiece). Fig. 1 Relationship between ferromagnetic resonance frequency f r and coercive field (H c ) of ε-ga x Fe 2-x O 3. f r and the H c values are related by f r = αh c (α = 9.63). 1.(1)-1) Angew. Chem. Int. Ed., 46, 8392 (2007). (highlighted at the Inside Cover). (2) Ferroelectric-ferromagnetic cyano-bridged metal assembly We have observed the coexistence of ferroelectricity and ferromagnetism in Rb 0.82 Mn[Fe(CN) 6 ] 0.94 H 2 O. The ferroelectricity is Fig. 3 The crystal structures of the prepared compound (a) before and (b) after adsorption of n-propanol. (3) Chemical-sensing magnet (Alcohol vapor) A copper(ii) octacyanotungsten(v)-based ferromagnet, Cu II 3[W V (CN) 8 ] 2 (pyrimidine) 2 8H 2 O, was prepared. This magnetic material can reversibly adsorb and desorb n-propanol vapor, and shows reversible variations in the crystal structure and magnetic properties. These changes are due to the coordination geometry switching of Cu II between 6-coordinate and 5-coordinate.
2 1.(1)-3) J. Am. Chem. Soc., 129, 3084 (2007). 物性化学研究室 研究ハイライト (1) イプシロン型 ガリウム酸化鉄からなるミリ波吸吸体イプシロン型 酸化鉄という特殊なナノ磁性体の鉄イオンの一部をガリウムイオンで置換した イプシロン型 ガリウム酸化鉄 ( ε -Ga x Fe 2-x O 3 ;0.10 < x < 0.67) ナノ微粒子 ( 粒径が 30 ナノメートル程度 ) を化学的に合成し ガリウム置換量に応じて 30GHz から 150GHz までの高い周波数領域でミリ波を有効かつ周波数選択的に吸収することを見出した また 理論計算によりこの系列の材料では ガリウム置換量により吸収可能な最大周波数は 200GHz までに達することが示された このミリ波吸収は イプシロン型 ガリウム酸化鉄磁性体がもつ高い保磁力により高い周波数に自然共鳴が現れたことに起因する イプシロン型 ガリウム酸化鉄は 金属酸化物であるため長期間に渡って安定である 電磁波干渉抑制材料として オフィスや医療室の壁への塗布のほか 車 電車 飛行機の胴体への塗布 また その選択的な共鳴周波数を用いてミリ波発信機を安定化させるサーキュレーターやアイソレターなどの新規ミリ波用電子デバイスへの応用も期待される Fig. 2 Rb 0.82 Mn[Fe(CN) 6 ] 0.94 H 2 O が示す強誘電性 ( 左図 ) および強磁性 ( 右図 ) 1.(1)-2) Angew. Chem. Int. Ed., 46, 3238 (2007). (highlighted in the frontispiece). (3) 化学的刺激 ( アルコール蒸気 ) に応答する磁性体化学的刺激に応答する磁性体の合成の一環として 1- プロパノール蒸気に可逆に応答する Cu II 3[W V (CN) 8 ] 2 (pyrimidine) 2 8H 2 O 強磁性体の合成に成功した 可逆な磁気特性変化は 1- プロパノール分子の吸着 脱離により Cu II の配位構造が 6 配位八面体構造と 5 配位四角錐構造の間でスイッチングすることに起因していることを単結晶構造解析から明らかにした Fig. 1 ε-ga x Fe 2-x O 3 における強磁性共鳴周波数 f r と保磁力 H c の関係 f r と H c は f r = αh c (α = 9.63) の関係式で結ばれる 1.(1)-1) Angew. Chem. Int. Ed., 46, 8392 (2007). (highlighted at the Inside Cover). (2) 強誘電 強磁性金属錯体シアノ架橋型金属錯体 Rb 0.82 Mn[Fe(CN) 6 ] 0.94 H 2 O において強誘電性と強磁性が共存することを見出した 強誘電性の起源は 鉄欠陥および Fe II, Fe III, Mn II, ヤーンテラーひずみを有する Mn III が混在することであり また強磁性の起源は Mn III のスピンが強磁性的相互作用により平行に整列していることで説明される Fig プロパノール吸着前 (a) および吸着後 (b) の Cu II 3[W V (CN) 8 ] 2 (pyrimidine) 2 の結晶構造
3 1.(1)-3) J. Am. Chem. Soc., 129, 3084 (2007). 1. 原著論文 (1) Refereed Journals 1) A millimeter-wave absorber based on gallium-substituted ε-iron oxide nanomagnets S. Ohkoshi, S. Kuroki, S. Sakurai, K. Matsumoto, K. Sato, and S. Sasaki Angew. Chem. Int. Ed., 46, (2007). (highlighted at the Inside Cover) 2) Coexistence of ferroelectricity and ferromagnetism in a rubidium manganese hexacyanoferrate S. Ohkoshi, H. Tokoro,T. Matsuda,T. Takahashi, H. Irie, and K. Hashimoto Angew. Chem. Int. Ed., 46, (2007).(highlighted in the frontispiece) 3) Synthesis and alcohol vapor sensitivity of a ferromagnetic copper-tungsten bimetallic assembly S. Ohkoshi, Y. Tsunobuchi, H. Takahashi, T. Hozumi, M. Shiro, and K. Hashimoto J. Am. Chem. Soc., 129, (2007). 4) Thermal spin transition investigated by spectroscopic ellipsometry in [Fe(NH 2 -trz) 3 ]Br 2 E. D. Loutete-Dangui, F. Varret, E. Codjovi, P. R. Dahoo, H. Tokoro, S. Ohkoshi, C. Eypert, J.F. Letard, J. M. Coanga, and K. Boukheddaden Phys. Rev. B, 75, /1-7 (2007). 5) Syhthesis,, and magnetic properties in ε-in x Fe 2-x O 3 nanorod-shaped magnets. S. Sakurai, S. Kuroki, H. Tokoro, K. Hashimoto, and S. Ohkoshi Adv. Funct. Mater., 17, (2007). 6) Piezomagnetic behavior of the spin crossover Prussian blue analogue CsFe[Cr(CN) 6 ] D. Papanikolaou, W. Kosaka, S. Margadonna, H. Kagi, S.Ohkoshi, and K. Prassides J. Phys. Chem. C, 111, (2007). 7) Photoinduced charge transfer phase transition in cesium manganese hexacyanoferrate T. Matsuda, H. Tokoro, K. Hashimoto, and S. Ohkoshi J. Appl. Phys., 101, 09E101/1-3 (2007). 8) Photo-induced charge transfer phase transition of manganese hexacyanoferrate in ferromagnetic and paramagnetic states H. Tokoro, K. Hashimoto, and S. Ohkoshi J. Mag. Mag. Mater., 310, (2007). 9) Charge-transfer transition in a two-dimensional Cs[Co(3-cyanopyridine) 2 ][W(CN) 8 ] H 2 O as investigated by angle-resolved x-ray diffraction J. Kim, Y. Moritomo, K. Kato, M. Takata, and S. Ohkoshi Phys. Rev. B, 76, /1-6 (2007). 10) Role of the intermediate state in the photoinduced process of Co-Fe cyanide Y. Moritomo, F. Nakada, H. Kamioka, T. Hozumi and S. Ohkoshi Phys. Rev. B, 75, /1-4 (2007). 11) Octacyanotungstate(IV)-Based Magnetic Complex Consisting of Dimeric Mn 2 and Tetrameric Mn 2 W 2 Z. X. Wang, X. L. Li, T. W. Wang, Y. Z. Li, S. Ohkoshi, K. Hashimoto, Y. Song and X. Z. You Inorg. Chem. 46, (2007) 12) A high compensation temperature of 175 K in a vanadium hexacyanochromate-based magnet S. Ohkoshi, T. Hozumi, M. Mizuno, and K. Hashimoto Chem Lett., 36, (2007). 13), Magnetic properties, and Second Harmonic Generation of a Three-dimensional Pyroelectryc Cyano-bridged Mn-Mo Complex W. Kosaka, T. Nuida, K. Hashimoto, and S. Ohkoshi Bull. Chem. Soc. Jpn., 80, (2007). 14) Single Crystal of a Prussian Blue Analog based on Rubidium Manganese Hexacyanoferrate H. Tokoro, M. Shiro, K. Hashimoto, and S. Ohkoshi Z. Anorg. Allg. Chem., 633, (2007). 15) Two-dimensional metamagnet composed of a cesium copper octacyanotungustate S. Kaneko, Y. Tsunobuchi, S. Sakurai, and S. Ohkoshi Chem. Phys. Lett., 446, (2007). 16) Calorimetric investigation of equilibrium and thermal relaxation properties of the switchable Prussian blue analog Na 0.32 Co[Fe(CN) 6 ] H 2 O
4 M. Castro, J. A. Rodriguez-Velamazan, K. Boukheddaden, F. Varret, H. Tokoro, and S. Ohkoshi Europhys. Lett., 79, 27007/1-6 (2007). 17) Substitution effects of barium and calcium on magnetic properties of AxSr 1-x (Fe 0.5 Ru 0.5 )O 3 double perovskites (x=0.05, A=Ba,Ca) K. Nomura, R. Zboril, J. Tucek,W. Kosaka, S. Ohkoshi, and I. Felner J. Appl. Phys., 102, /1-11 (2007). 18) Observation of a phase transition of cesium manganese hexacyanoferrates by x-ray absorption spectroscopy K. Ishii, T. Matsuda, H. Tokoro, T. Iwazumi, K. Hashimoto, and S.Ohkoshi J. Phys. Chem. Solid., 68, (2007). 19) Poly[[diaquahexa-μ-cyanido-dicyanido-di-μ-pyrimidine-dimanganese(II)molybdate (IV)]trihydrate] W. Kosaka, K. Hashimoto, and S. Ohkoshi Acta Cryst. E, 63, m1220-m1222 (2007). 20) Cyano-bridged gadolinium-tungstate bimetallic one-dimensional chains with a dimethylacetamide ligand W. Kosaka, K. Hashimoto, and S. Ohkoshi Bull. Chem. Soc. Jpn., 80, 12, (2007). 21) Nonlinear magneto-optical effects and photomagnetism of electrochemically synthesized molecule-based magnets T. Nuida, T. Hozumi, H. Tokoro, K. Hashimoto, and S. Ohkoshi J. Solid State Electrochem., 11, (2007). 22) Poly[triaquaocta-m-cyano-dicopper(II)molybdate(IV)monohydrate] Y. Zhang, T. Hozumi, K. Hashimoto, and S. Ohkoshi Acta Cryst. E, 63, i30-i32 (2007). 23) Manipulating the through-space spin-spin interaction of organic radicals in the confined cavity of a self-assembled cage K. Nakabayashi, M. Kawano, T. Kato, K. Furukawa, S. Ohkoshi, T. Hozumi, and M. Fujita Chem. Asian. J., 2, (2007). 24) Extended charge-transfer state of RbMn[Fe(CN) 6 ] K. Kato, Y. Moritomo, H. Tanaka, H. Tokoro, S. Ohkoshi, and M. Takata J. Phys. Soc. Jpn., 76, /1-3 (2007). 25) Porous magnets based on copper-octacyanotungsten containing noncoordinated alcohol molecules Y. Tsunobuchi, K. Hashimoto, M. Shiro, T. Hozumi, and S. Ohkoshi Chem Lett., 36, (2007). 2. 総説 解説 1) 特定領域研究配位空間の化学 広報 8, 3 (2007). 3. 著書 4. その他 1) 朝日新聞 (2007 年 10 月 26 日 )(37 面 ) 次世代通信の要 電磁波さえぎる新素材 2) 毎日新聞 (2007 年 11 月 4 日 )(25 面 ) ミリ波 高周波の波吸収する新材料開発東大 大越教授ら 3) 日経産業新聞 (2007 年 10 月 26 日 )(8 面 ) 150 ギガヘルツ超の電波に対応 4) 日刊工業新聞 (2007 年 10 月 26 日 )(26 面 ) 150 ギガヘルツ帯域のミリ波吸収 5) 毎日 jp (2007 年 11 月 4 日 ) 新材料 : ミリ波 高周波の波を吸収東大 大越教授ら開発 6) 東大新聞 (2007 年 11 月 20 日 ) 大越教授ら 150 ギガヘルツ吸収素材開発 [ 特許 ] 1) 大越慎一, 他 5 名, 国際出願 PCT/JP2007/ ) 大越慎一, 他 3 名, 米国特許出願 US11/521, 395 3) 大越慎一, 他 4 名, 欧州特許出願 ) 大越慎一, 他 4 名, 中国特許出願 X 5) 大越慎一, 他 4 名, 国際出願 PCT/JP2007/067351
5 6) 大越慎一, 他 4 名, 米国特許出願 US11/892, 911 7) 大越慎一, 他 2 名, 特願 ) 大越慎一, 他 4 名, 特願 ) 大越慎一, 他 4 名, 特願 ) 大越慎一, 他 1 名, 特願 ) 大越慎一, 他 5 名, 特願 ) 大越慎一, 他 4 名, 特願 ) 大越慎一, 他 1 名, 特願
2. 研究実施内容 ( 文中に番号がある場合は (3-1) に対応する ) 研究のねらい本研究では 磁気化学を基盤とした新機能ナノ構造物質のボトムアップ創成に関する研究を推進している 目的としては 金属錯体磁性体の高次構造を制御することで 新規光磁性材料の創製や 優れた磁気特性などの新規機能性を有す
プロセスインテグレーションに向けた高機能ナノ構造体の創出 平成 22 年度採択研究代表者 H23 年度 実績報告 大越慎一 東京大学大学院理学系研究科 教授 磁気化学を基盤とした新機能ナノ構造物質のボトムアップ創成 1. 研究実施体制 (1) 大越グループ 1 研究代表者 : 大越慎一 ( 東京大学大学院理学系研究科 教授 ) 2 研究項目 1. 磁性金属錯体に関する研究 (i) 新規光磁性金属錯体のボトムアップ合成
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