Search for new rattling materials, crystal growth, and study of electron-phonon properties

2012 Fiscal Year Final Research Report

• Project Area: Emergence of Heavy Electrons and Their Ordering
• Project/Area Number: 20102004
• Research Category: Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
• Allocation Type: Single-year Grants
• Review Section: Science and Engineering
• Research Institution: Hiroshima University
• Principal Investigator: TAKABATAKE Toshiro 広島大学, 大学院・先端物質科学研究科, 教授 (40171540)
• Co-Investigator(Kenkyū-buntansha): SUGAWARA Hitoshi 神戸大学, 大学院・理学研究科, 教授 (60264587) ; SEKINE Chihiro 室蘭工業大学, 工学研究科, 教授 (60261385) ; TAKEDA Naoya 新潟大学, 自然科学系, 教授 (80242171) ; IGA Fumitoshi 茨城大学, 理学部, 教授 (60192473)
• Co-Investigator(Renkei-kenkyūsha): HIROI Zenji 東京大学, 物性研究所, 教授 (30192719)
• Project Period (FY): 2008 – 2012
• Keywords: クラスレート / ラットリング / 重い電子系化合物 / 電子・格子相互作用 / 結晶育成 / 超高圧合成

Research Abstract

New class of compounds showing rattling and related phenomena has been synthesized. (1) The off-center rattling of Ba guests in Ba_8Ga_<16>Sn_<30> enhances the specific heat coefficient and reduces the thermal conductivity. (2) The anomalous phase transition in CeT_2Al_<10> (T=Ru, Os) is an antiferromagnetic order in the partially gapped state. The La counterparts have a three dimensional multiply-connected Fermi surface. (3) The rattling energy of the As-based skutterudites is between those for P-based and Sb-based systems. (4) Among heavy rare-earth filled R_5T_6Sn_<18> (T=Co, Ir), Lu_5Ir_6Sn_<18> shows superconductivity at 2.6 K. (5) The coupling of acoustic phonons and magnetic excitations plays an essential role in the formation of the gap in YbB_<12>.

Research Products

• [Journal Article] Anomalous infrared spectra of hybridized phonons in type-I clathrate Ba_8Ga_<16>Ge_<30> (2013)
  • Author(s): K. Iwamoto, S. Kushibiki, H. Honda, S. Kajitani, T. Mori, H. Matsumoto, N. Toyota, K. Suekuni, M. A. Avila, T. Takabatake
  • Journal Title: J. Phys. Soc. Jpn Volume: 82 Pages: 024601/1-7
  • Peer Reviewed
• [Journal Article] Severing, Crystal field ground state of the orthorhombic Kondo semiconductors CeOs_2Al_<10> and CeFe_2Al_<10> (2013)
  • Author(s): F. Strigari, T. Willers, Y. Muro, K. Yutani, T. Takabatake, Z. Hu, S. Agrestini, C.-Y. Kuo, Y.-Y. Chin, H.-J. Lin, T. W. Pi, C. T. Chen, E. Weschke, E. Schierle, A. Tanaka, M. W. Haverkort, L. H. Tjeng, A
  • Journal Title: Phys. Rev. B Volume: 87 Pages: 125119/1-6
  • Peer Reviewed
• [Journal Article] High-field phase diagram of SmRu_4P_<12> determined by ultrasonic measurements in pulsed magnetic field up to 55 T (2013)
  • Author(s): M. Yoshizawa, H. Mitamura, F. Shichinomiya, S. Fukuda, Y. Nakanishi, H. Sugawara, T. Sakakibara, K. Kindo
  • Journal Title: J. Phys. Soc. Jpn Volume: 82 Pages: 033602/1-5
  • Peer Reviewed
• [Journal Article] Pressure-temperature phase diagram of Sm valence state in a heavy fermion compound SmOs_4Sb_<12> (2013)
  • Author(s): S. Tsutsui, N. Kawamura, M. Mizumaki, N. Ishimatsu, H. Maruyama, H. Sugawara and H. Sato
  • Journal Title: J. Phys. Soc. Jpn Volume: 82 Pages: 023707/1-4
  • Peer Reviewed
• [Journal Article] Low-temperature magnetic properties of RE_2Ni_<21>B_6 (RE=Er,Tm,Yb and Lu) (2013)
  • Author(s): J. Kitagawa, N. Takeda and M. Ishikawa
  • Journal Title: J. Alloys and Compd Volume: 561 Pages: 101-104
  • Peer Reviewed
• [Journal Article] Magnetic phase diagram of clathrate compound Ce_3Pd_<30>Si_6 with quadrupolar ordering (2013)
  • Author(s): H. Ono, T. Nakano, N. Takeda, G. Ano, M. Akatsu, Y. Nemoto, T. Goto, A. Donni and H. Kitazawa
  • Journal Title: J. Phys. : Condens. Matter Volume: 25 Pages: 126003/1-4
  • Peer Reviewed
• [Journal Article] Well-defined crystal field splitting schemes and non-Kramers doublet ground states of f electrons in PrT_2Zn_<20> (T=Ir, Rh, and Ru), (2013)
  • Author(s): K. Iwasa, H. Kobayashi, T. Onimaru, K. T. Matsumoto, N. Nagasawa, T. Takabatake, S. Ohira-Kawamura, T. Kikuchi, Y. Inamura, K. Makajima
  • Journal Title: J. Phys. Soc. Jpn Volume: 82 Pages: 043707/1-5
  • Peer Reviewed
• [Journal Article] Study of α⇔β transformation in the dimorphic clathrate Ba_8Ga_<16>Sn_<30> (2012)
  • Author(s): B. Du, Y. Saiga, K. Kajisa, T. Takabatake, E. Nishibori, H. Sawa
  • Journal Title: Phil. Magaz Volume: 92 Pages: 2541-2552
  • Peer Reviewed
• [Journal Article] Lattice instability and elastic dispersion due to the rattling motion in the type-I clathrate Ba_8Ga_<16>Sn_<30> (2012)
  • Author(s): I. Ishii, Y. Suetomi, T. K. Fujita, K. Suekuni, T. Tanaka, T. Takabatake, T. Suzuki, M. A. Avila
  • Journal Title: Phys. Rev. B Volume: 85 Pages: 085101(1-7)
  • Peer Reviewed
• [Journal Article] Effects of filling fraction on magnetic properties of filled skutterudite Rfe_4Sb_<12> (R = La, Ce) synthesized under high pressure (2012)
  • Author(s): K. Magishi, H. Sugawara, M. Takahashi, T. Saito, K. Koyama, T. Saito, S. Tatsuoka, K. Tanaka, H. Sato
  • Journal Title: J. Phys. Soc. Jpn Volume: 81 Pages: 124706/1-5
  • Peer Reviewed
• [Journal Article] Penetration depth study of LaOs_4Sb_<12>: Multiband s-wave superconductivity (2012)
  • Author(s): X.Y. Tee, H.G. Luo, T. Xiang, D. Vandervelde, M.B. Salamon, H. Sugawara, H. Sato, C. Panagopoulos, E.E.M. Chia
  • Journal Title: Phys. Rev. B Volume: 86 Pages: 064518/1-5
  • Peer Reviewed
• [Journal Article] Ferromagnetic ground states with high transition temperatures in new tetragonal rare-earth compounds CeRu_2A_<l2>B and PrRu_2A_<l2>B (2012)
  • Author(s): E. Matsuoka, Y. Tomiyama, H. Sugawara, T. Sakurai, H. Ohta
  • Journal Title: J. Phys. Soc. Jpn Volume: 81 Pages: 043704/1-4
  • Peer Reviewed
• [Journal Article] Structural instability of unfilled skutterudite compounds MX_3 (M = Co, Rh, and Ir; X = As and Sb) under high pressure (2012)
  • Author(s): K. Matsui, K. Yamamoto, T. Kawai, Y. Kawamura, J. Hayashi, K. Takeda, C. Sekine
  • Journal Title: J. Phys. Soc. Jpn Volume: 81 Pages: 104604/1-7
  • Peer Reviewed
• [Journal Article] ^<149>Sm and ^<57>Fe nuclear resonant inelastic scattering of filled skutterudites SmFe_4X_<12> (X: Pnictogen) (2012)
  • Author(s): S. Tsutsui, H. Kobayashi, Y. Yoda, H. Sugawara, C. Sekine, T. Namiki, I. Shirotani, H. Sato
  • Journal Title: Hyperfine Interactions Volume: 206 Pages: 67-70
  • Peer Reviewed
• [Journal Article] Pressure suppression of unconventional charge-density-wave state in PrRu_4P_<12> studied by optical conductivity (2012)
  • Author(s): H. Okamura, N. Ohta, A. Takigawa, I. Matsutori, K. Shoji, K. Miyata, M. Matsunami, T. Nanba, H. Sugawara, C. Sekine, I. Shirotani, H. Sato, T. Moriwaki, Y. Ikemoto, Z. Liu, G. L. Carr
  • Journal Title: Phys. Rev. B Volume: 85 Pages: 205116/1-7
  • Peer Reviewed
• [Journal Article] Magnetization, resistivity and specific heat of hexagonal R_2Ni_<12>P_7 with filled-Cr_<12>P_7 structure (2012)
  • Author(s): T. Nakano, K. Tsuchiya, A. Ohashi, T. Nashimoto, H. Ono, N. Takeda, N. Shirakawa
  • Journal Title: J. Phys. Soc. Jpn Volume: 81 Pages: 074601/1-8
  • Peer Reviewed
• [Journal Article] Interplay of low-energy phonons and magnetic excitations in the Kondo insulator YbB_<12> (2012)
  • Author(s): P. V. Alekseev, J-M. Mignot, K. S. Nemkovski, A. V. Rybina, V. N. Lazukov, A. S. Ivanov, F. Iga, T. Takabatake
  • Journal Title: J. Phys.: Cond. Matter Volume: 24 Pages: 205601/1-5
  • Peer Reviewed
• [Journal Article] Antiferroquadrupole order and magnetic field induced octupole in CeB_6 (2012)
  • Author(s): T. Matsumura, T. Yonemura, K. Kunimori, M. Sera, F. Iga, T. Nagao, J. Igarashi
  • Journal Title: Phys. Rev. B Volume: 85 Pages: 174417(1-10)
  • Peer Reviewed
• [Journal Article] New type of the domain-redistribution at low magnetic fields in phase II of CeB_6 (2012)
  • Author(s): K. Kunimori, M. Sera, H. Tanida, T. Matsumura, F. Iga
  • Journal Title: J. Phys. Soc. Japan Volume: 81(10) Pages: 104706/1-6
  • Peer Reviewed
• [Journal Article] Quadrupole ordering and ruttling motion of clathrate compound Pr_3Pd_<20>Ge_6 (2012)
  • Author(s): G. Ano, M. Akatsu, K. Araki, K. Matsuo, Y. Tchikawa, K. Mitsumoto, T. Yamaguchi, Y. Nemoto, T. Goto, N. Takeda, A. Donni, H. Kiatazawa
  • Journal Title: J. Phys. Soc. Jpn Volume: 81 Pages: 034710/1-11
  • Peer Reviewed
• [Journal Article] Electronic- structure-driven magnetic ordering in a Kondo semiconductor CeOs_2Al_<10> (2011)
  • Author(s): S. Kimura, T. Iizuka, H. Miyazaki, A. Irizawa, Y. Muro, T. Takabatake
  • Journal Title: Phys. Rev. Lett Volume: 106 Pages: 056404/1-4
  • Peer Reviewed
• [Journal Article] Antiferroquadrupolar ordering in a Pr-based superconductor PrIr_2Zn_<20> (2011)
  • Author(s): T. Onimaru, K. T. Matsuomoto, Y. F. Inoue, K. Umeo, T. Sakakibara, Y. Karaki, M. Kubota, T. Takabatake
  • Journal Title: Phys. Rev. Lett Volume: 106 Pages: 177001/1-4
  • Peer Reviewed
• [Journal Article] Pressure effect on the anomalous phase transition in CeOs_2Al_<10> (2011)
  • Author(s): K. Umeo, T. Ohsuka, Y Muro, J. Kajino, T. Takabatake
  • Journal Title: J. Phys. Soc. Jpn Volume: 80 Pages: 064709 /1-5
  • Peer Reviewed
• [Journal Article] Off-center rattling and thermoelectric properties of type-II clathrate (K,Ba)_<24>(Ga, Sn,□ )_<136> single crystals (2011)
  • Author(s): S. Mano, T. Onimaru, S. Yamanaka, T. Takabatake
  • Journal Title: Phys. Rev. B Volume: 84 Pages: 214101/1-6
  • Peer Reviewed
• [Journal Article] de Haas-van Alphen effect in SmOs_4P_<12> (2011)
  • Author(s): S. Tanaka, M. Sakoda, E. Matsuoka, H. Sugawara, R. Settai and Y. O^^-nuki
  • Journal Title: J. Phys.: Conf. Ser Volume: 273 Pages: 012060/1-4
  • Peer Reviewed
• [Journal Article] Rare-earth dependence of Einstein temperatures in filled skutterudite compounds REFe_4P_<12> (RE = La, Ce, Pr, Nd, and Sm) (2011)
  • Author(s): M. Mizumaki, S. Tsutui, T. Uruga, H. Tanida, D. Kikuchi, H. Sugawara, H. Sato
  • Journal Title: J. Phys. Soc. Jpn Volume: 80 Pages: 074603 /1-6
  • Peer Reviewed
• [Journal Article] Possible mass enhancement by multipole fluctuations excited via the singlet-triplet crystal electric field states in PrOs_4Sb_<12>: Sb-NMR studies using a single crystal (2011)
  • Author(s): H. Tou, Y. Inaoka, M. Doi, M. Sera, K. Asaki, H. Kotegawa, H. Sugawara, H. Sato
  • Journal Title: J. Phys. Soc. Jpn Volume: 80 Pages: 074703/1-17
  • Peer Reviewed
• [Journal Article] Magnetic phase diagram of (Pr_<1-x>Ce_x)Ru_4P_<12> (2011)
  • Author(s): C. Sekine, M. Takusari, T. Yagi
  • Journal Title: J. Phys. Soc. Jpn Volume: 80 Pages: SA024/1-3
  • Peer Reviewed
• [Journal Article] ^<31>P nuclear magnetic resonance and ^<101>Ru nuclear quadrupole resonance measurements of filled skutterudites GdRu_4P_<12> and TbRu_4P_<12> (2011)
  • Author(s): H. Fukazawa, R. Kobayashi, M. Shimizu, H. Amanuma, K. Hachitani, Y. Komaki, Y. Kohori, K. Akahira, C. Sekine and I. Shirotani
  • Journal Title: J. Phys. Soc. Jpn Volume: 80 Pages: 044713/1-5
  • Peer Reviewed
• [Journal Article] Motion of the guest ion as precursor to the first-order phase transition in the cage system GdB_6 (2011)
  • Author(s): K. Iwasa, R. Igarashi, K. Saito, C. Laulhe, T. Orihara, S. Kunii, K. Kuwahara, H. Nakao, Y. Murakami, F. Iga, M. Sera, S. Tsutsui, H. Uchiyama, A. Q. R. Baron
  • Journal Title: Phys. Rev. B Volume: 84 Pages: 214308(1-6)
  • Peer Reviewed
• [Journal Article] Off-center modes and glasslike thermal conductivity in the type-I clathrate Ba_8Ga_<16>Sn_<30> (2010)
  • Author(s): K. Suekuni, Y. Takasu, T. Hasegawa, N. Ogita, M. Udagawa, M. A. Avila, T. Takabatake
  • Journal Title: Phys. Rev. B Volume: 81 Pages: 205207/1-5
  • Peer Reviewed
• [Journal Article] Ferrimagnetism of new filled skutterudite SmFe_4As_<12> synthesized at high pressure (2010)
  • Author(s): T. Namiki, C. Sekine, K. Matsuhira, M. Wakeshima, I. Shirotani
  • Journal Title: J. Phys. Soc. Jpn Volume: 79 Pages: 074714/1-4
  • Peer Reviewed
• [Journal Article] X-ray atomic orbital analysis of 4f and 5d electron configuration of SmB_6 at 100, 165, 230 and 298 K (2010)
  • Author(s): S. Funahashi, K. Tanaka, F. Iga
  • Journal Title: Acta Cryst. B Volume: 66 Pages: 292-306
  • Peer Reviewed
• [Journal Article] Quadrupole ordering in clathrate compound Ce_3Pd_<20>Si_6 (2009)
  • Author(s): T. Goto, T. Watanabe, S. Tsuduku, H. Kobayashi, Y. Nemoto, T. Yanagisawa, M. Akatsu, G. Ano, O. Suzuki, N. Takeda, A. Donni, H. Kitazawa
  • Journal Title: J. Phys. Soc. Jpn Volume: 78 Pages: 024716/1-5
  • Peer Reviewed
• [Journal Article] Rattling-induced superconductivity in the .-pyrochlore oxides Aos_2O_6 (2009)
  • Author(s): Y. Nagao, J. Yamaura, H. Ogusu, Y. Okamoto, Z. Hiroi
  • Journal Title: J. Phys. Soc. Jpn Volume: 78 Pages: 064702/1-21
  • Peer Reviewed
• [Presentation] Recent advances in Ba-Ga-Sn based thermoelectric clathrates (2012)
  • Author(s): T. Takabatake
  • Organizer: 31^<th> Intern. & 10^<th> European Conf. on Thermoelectrics
  • Place of Presentation: Aalborg,デンマーク
  • Year and Date: 2012-07-11
• [Presentation] Physical properties of unfilled skutterudite NiP_3 (2010)
  • Author(s): 武田直也, 他4名
  • Organizer: Intern. Conf. on Heavy Electrons 2010
  • Place of Presentation: 首都大学東京, 八王子市
  • Year and Date: 2010-09-18
• [Presentation] Magnetic properties of new filled skutterudite compounds GdFe_4As_<12> and TbFe_4As_<12> (2010)
  • Author(s): 関根ちひろ,他3名
  • Organizer: Intern. Conf. Strongly Correlated Electron Systems
  • Place of Presentation: Santa Fe, USA
  • Year and Date: 2010-06-29
• [Presentation] Magnetic order in a heavy fermion state of Yb^<2+>_<1-x>TmxB_6 (2010)
  • Author(s): 伊賀文俊, 他8名
  • Organizer: Intern. Conf. Strongly Correlated Electron Systems
  • Place of Presentation: Santa Fe, USA
  • Year and Date: 2010-06-29
• [Presentation] Raman study of crystal electric field excitations in PrRu_4P_<12> (2010)
  • Author(s): N. Ogita, T. Hasegawa,菅原仁, H. Sato, M. Udagawa
  • Organizer: Intern. Conf. Strongly Correlated Electron Systems
  • Place of Presentation: Santa Fe, USA
  • Year and Date: 2010-06-28
• [Presentation] Thermoelectric clathrates with off-center ratting ions (2010)
  • Author(s): T. Takabatake
  • Organizer: ICT2010 (国際熱電学会)
  • Place of Presentation: 上海, 中国
  • Year and Date: 2010-05-31
• [Book] 監修 梶川武信河本邦仁,熱電学熱電材料と製造プロセス技術第2章第5節クラスレート材料と単結晶育成 (2012)
  • Author(s): 高畠敏郎
  • Total Pages: 370, 111-124
  • Publisher: サイエンス&テクノロジー
• [Book] 熱電変換技術の基礎と応用(第4章)編纂日本熱電学会,クラスレート化合物 (2011)
  • Author(s): 高畠敏郎
  • Total Pages: 251, 66-71
• [Book] North-Holland, Handbook of Magnetic Materials, Vol.18, Chap. 1, Magnetic properties of filled skutterudites, ed. by K. H. J. Buschow (2009)
  • Author(s): H. Sato, H. Sugawara, Y. Aoki, H. Harima
  • Total Pages: 1-110
  • Publisher: Elsevier
• [Remarks]
  • URL: http://www.heavy-electrons.jp/
• [Patent(Industrial Property Rights)] クラスレート化合物,熱電変換材料,およびそれらの製造方法 (2011)
  • Inventor(s): 河野欽,田口隆志,高畠敏郎,才賀裕太,デン スーカン
  • Industrial Property Rights Holder: 国立大学法人広島大学,株式会社デンソー
  • Industrial Property Number: 特願 2011-86395
  • Filing Date: 2011-04-08
• [Patent(Industrial Property Rights)] クラスレート化合物,熱電変換材料,およびそれらの製造方法 (2010)
  • Inventor(s): 河野欽,田口隆志,大矢信之,高畠敏郎,才賀裕太,デン スーカン
  • Industrial Property Rights Holder: 国立大学法人広島大学,株式会社デンソー
  • Industrial Property Number: 特願 2010-108524
  • Filing Date: 2010-05-10