The Physics and Chemistry of Organic Superconductors Proceedings of the ISSP International Symposium, Tokyo, Japan, August 28 - 30,1989

Editors: G.Saito and S.Kagoshima

With 300 Figures

Springer-Verlag Berlin Heidelberg NewYork London Paris Tokyo Hong Kong

Contents

Part I Organic Superconductors: Overview and Comparison with Oxide Superconductors

Recent Developments in Organic Superconductors By D. Jerome, P. Auban, W. Kang, and J.R. Cooper (With 4 Figures) . . 2 Trends in Structures and Properties of Organic and Inorganic Superconductors By P. Day (With 4 Figures) 8 On Some Organic Conductors in the Light of Oxide Superconductors By H. Fukuyama (With 3 Figures) 15

Part П Metal Coordinated Organic Conductors and Related Materials

Conductive and Superconductive Coordination Compounds By P. Cassoux, L. Valade, J.-P. Legros, С Tejel, J.-P. Ulmet, and L. Brossard (With 3 Figures) 22 Synthesis and Properties of the New Molecular Metals Na[Ni(dmit)2]2 and NH4[Ni(dmit)2]2 By R.A. Clark, A.E. Underbill, R. Friend, M. Allen, I. Marsden, A. Kobayashi, and H. Kobayashi (With 3 Figures) 28 Effect of Counter Ions on Alkali Metal Salts of MztNKdmif^] (M=Na, NH4...) By A. Izuoka, A. Miyazaki, N. Sato, T. Sugawara, and T. Enoki (With 1 Figure) 32 The Organic 7r-Electron Metal System Interacting with Mixed-Valence Copper Ions (R1,R2-DCNQr)2Cu (DCNQI=N,N'-dicyanoquinonediimine; R1 ,R2 = CH3, CH30, Cl, Br) By R. Kato, H. Kobayashi, and A. Kobayashi (With 4 Figures) 36 Metallic DCNQI Salts: Influence of Oxygen, Alloying and Dimensionality By M. Bair, U. Langohr, J.U. von Schütz, H.C. Wolf, P. Erk, H. Meixner, and S. Hünig (With 2 Figures) 41

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Anomalous Temperature Dependence of the Resistivity of (DMeO-DCNQI)2Cu at High Pressure By H. Kobayashi, A. Miyamoto, R. Kato, Y. Nishio, K. Kajita, W. Sasaki, and A. Kobayashi (With 3 Figures) 45

Reflectance Spectra of DCNQI Salts By H. Tajima, G. Ojima, T. Ida, H. Kuroda, A. Kobayashi, R. Kato, H. Kobayashi, A. Ugawa, and K. Yakushi (With 5 Figures) 49

Optical Spectra of Highly Conducting Phthalocyanine Salts By K. Yakushi, H. Yamakado, T. Ida, A. Ugawa, H. Masuda, and H. Kuroda (With 3 Figures) 54

Preparation of Electroconducting Materials Containing Copper Compounds: A Copper Oxide with l,3,4,6-Tetrathiapentalene-2,5-dione By M. Inoue, C. Cruz-Väzquez, M.B. Inoue, K.W. Nebesny, and Q. Fernando (With 3 Figures) 58

Part П1 TMTSF Family: Superconductivity and Spin Density Waves

A Hidden Low-Temperature Phase in the Organic Conductor (TMTSF)2Re04 By S. Tomic and D. Jerome (With 3 Figures) 64 NMR Evidence for the Existence of ID Paramagnons in Organic Conductors By P. Wzietek, F. Creuzet, С Bourbonnais, D. Jerome, P. Batail, and K. Bechgaard (With 2 Figures) 68 Long-Range Spin-Fluctuations and Superconductivity in the Quasi-One-Dimensional Hubbard Model By H. Shimahara (With 2 Figures) 73

Transport Properties of Impure Anisotropic Quasi-One-Dimensional Superconductors By Y. Suzumura (With 3 Figures) 77 Some Recent Experiments on the Field Induced Spin Density Wave States in the Bechgaard Salts By P.M. Chaikin, J.S. Brooks, S.T. Hannahs, W. Kang, G. Montambaux, and L.Y. Chiang (With 2 Figures) 81 Phase Diagram of the Spin Density Waves Induced by the Magnetic Field in Organic Metals By F. Pesty, P. Garoche, and M. Heritier (With 2 Figures) 87 Spin Density Wave and Field Induced Spin Density Wave Transport By K. Maki (With 1 Figure) 91 Magnetothermodynamics and Magnetotransport in (TMTSF)2C104 By G. Montambaux (With 3 Figures) 97

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Quantized Hall Effect in Spin-Wave Phases of Two-Dimensional Conductors By M. Kohmoto 102 J H Spin-Lattice Relaxation in the SDW State of (TMTSF)2PF6 Under Pressure By T. Takahashi, T. Ohyama, T. Harada, K. Kanoda, K. Murata, and G. Saito (With 3 Figures) 107

Non-ohmic Electrical Transport in the Spin-Density Wave State of Organic Conductors By S. Tomic, J.R. Cooper, W. Kang, and D. Jerome (With 3 Figures) . . I l l

Part IV BEDT-TTF Family: Superconductivity

Superconductivity in BEDT-TTF Based Organic Metals: An Overview By M. Tokumoto (With 1 Figure) 116

T-P Phase Diagram of /3-(ET)2I3

By V.N. Laukhin, V.B. Ginodman, A.V. Gudenko, P.A. Kononovich, and I F . Schegolev (With 3 Figures) 122

"2K-Superconducting State" in the Organic Superconductor /HBEDT-TTF)2I3

By S. Kagoshima, M. Hasumi, Y. Nogami, N. Kinoshita, H. Anzai, M. Tokumoto, and G Saito (With 3 Figures) 126

A Change of the Incommensurate Superstructure in the Organic Superconductor /3-(BEDT-TTF)2I3

By Y. Nogami, S. Kagoshima, H. Anzai, M. Tokumoto, G. Saito, and N. Mori (With 3 Figures) 130

Effect of Annealing on the Superconductivity of /3-(BEDT-TTF)2I3

By K. Kanoda, K. Akiba, K. Suzuki, T. Takahashi, and G. Saito (With 2 Figures) 134

Evolution of the "High-Tc" States at Ambient Pressure in /3-(BEDT-TTF)2I3

By M. Tokumoto, Y. Yamaguchi, N. Kinoshita, and H. Anzai (With 3 Figures) 138

Electrical Resistance and Upper Critical Field in the "2K-Superconducting State" of /3-(BEDT-TTF)2I3

By T. Sasaki, N. Toyota, M. Hasumi, T. Osada, S. Kagoshima, M. Tokumoto, N. Kinoshita, and H. Anzai (With 2 Figures) 142

Bulk Superconductivity at Ambient Pressure in Polycrystalline Pressed Samples of Organic Metals By D. Schweitzer, S. Kahlich, S. Gärtner, E. Gogu, H. Grimm, R. Zamboni, and H.J. Keller (With 2 Figures) 146

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An Ambient Pressure Organic Superconductor K-(BEDT-TTF-hg and -d8)2Cu(NCS)2 with Tc Higher than 10K By H. Mori, S. Tanaka, H. Yamochi, G. Saito, and K. Oshima (With 5 Figures) 150 Nuclear Spin-Lattice Relaxation in the Organic Superconductor (BEDT-TTF)2Cu(NCS)2: Measurements by the Field Cycling Technique By T. Takahashi, K. Kanoda, K. Sakao, M. Watabe, H. Mori, and G. Saito (With 3 Figures) 155 Magnetic-Field Penetration Depth of (BEDT-TTF)2Cu(NCS)2 Determined by Complex Susceptibility By K. Kanoda, K. Akiba, T. Takahashi, and G. Saito (With 1 Figure) . . 159 Tunneling Spectroscopic Study of the Superconducting Gap of (BEDT-TTF)2Cu(NCS)2 Crystals By Y. Maruyama, T. Inabe, H. Mori, H. Yamochi, and G. Saito (With 4 Figures) 163 STM Measurements of Superconducting Properties in K-(BEDT-TTF)2Cu(NCS)2 By H. Bando, S. Kashiwaya, T. Tokumoto, H. Anzai, N. Kinoshita, M. Tokumoto, K. Murata, and K. Kajimura (With 2 Figures) 167 Effect of Tensile Stress on the Superconducting Transition Temperature in (BEDT-TTF)2Cu(NCS)2 By H. Kusuhara, Y. Sakata, Y. Ueba, K. Tada, M. Kaji, and T. Ishiguro (With 4 Figures) 171 Highly Correlated Fermi Liquids in the High-Tc Organic Conductor к-(BEDT-TTF)2Cu(NCS)2 By N. Toyota, E.W. Fenton, T. Sasaki, and M. Tachiki 177

Electronic Properties of (BEDT-TTF)3C12-2H20 By S.D. Obertelli, I.R. Marsden, R.H. Friend, M. Kurmoo, M.J. Rosseinsky, P. Day, F.L. Pratt, and W. Hayes (With 3 Figures) . . . 181

Part V BEDT-TTF Family: Fermiology and Related Subjects

Galvanomagnetic Properties of the Organic Metals /3-(ET)2X: Magnetoresistance and Shubnikov-de Haas Oscillations By V.N. Laukhin, M.V. Kartsovnik, S.I. Pesotskii, I.F. Schegolev, and P.A. Kononovich (With 5 Figures) 186 The Fermi Surface in the Organic Superconductor /3-(BEDT-TTF)2IBr2 By T. Sasaki, N. Toyota, T. Fukase, K. Murata, M. Tokumoto, and H. Anzai (With 4 Figures) 191 On the Electronic Properties of ET2Cu(NCS)2 as well as of Some New Organic Salts By H. Müller, С.-P. Heidmann, A. Lerf, W. Biberacher, R. Sieburger, and K. Andres (With 4 Figures) 195

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Fermi Surface and Band Structure of K - ( B E D T - T T F ) 2 C U ( N C S ) 2

By F.L. Pratt, J. Singleton, M. Kurmoo, S J.R.M. Spermon, W. Hayes, and P. Day (With 1 Figure) 200

Fermi Surface and Thermoelectric Power of Two-Dimensional Organic Conductors By T. Mori and H. Inokuchi (With 1 Figure) 204

Self-Consistent Band Structure and Fermi Surface for /3-(BEDT-TTF)2I3 By J. Kubier and C.B. Sommers (With 7 Figures) 208

Anomalous Magneto-oscillation in 0-Type Crystals of (BEDT-TTF)2I3 By K. Kajita, Y. Nishio, T. Takahashi, W. Sasaki, R. Kato, H. Kobayashi, A. Kobayashi, and Y. lye (With 6 Figures) 212

Nearly Complete Quantization in Quasi-Two-Dimensional Organic Superconductors By K. Yamaji (With 4 Figures) 216

High-Field Magnetotransport in the Organic Conductor (BEDT-TTF)2KHg(SCN)4

By T. Osada, R. Yagi, S. Kagoshima, N. Miura, M. Oshima, and G. Saito (With 4 Figures) 220

Electronic Properties in (BEDT-TTF)2X: Magnetoresistance and Hall Effect By K. Murata, M. Ishibashi, Y. Honda, T. Komazaki, M. Tokumoto, N. Kinoshita, and H. Anzai (With 3 Figures) 224

Part VI DMET Salts and Their Families

Physical Properties and Crystal Structures of DMET Superconductors and Conductors By K. Kikuchi, K. Murata, K. Saito, K. Kobayashi, and I. Dcemoto (With 4 Figures) 230

Superconductivity and Spin Density Waves in (DMET)2Au(CN)2 By K. Murata, K. Kikuchi, Y. Honda, T. Komazaki, K. Saito, K. Kobayashi, and I. Dcemoto (With 3 Figures) 234

Phase Transition of the Organic Metal (DMET)2Au(CN)2 at 180 К By K. Saito, K. Kikuchi, K. Kobayashi, and I. Dcemoto (With 4 Figures) 238

Antiferromagnetic Transitions in (DMET)2X and (DMPT)2X By K. Kanoda, S. Okui, T. Takahashi, K. Kikuchi, K. Saito, I. Dcemoto, and K. Kobayashi (With 2 Figures) 242

Conducting and Superconducting Salts Based on MDTTTF, EDTTTF, VDTTTF, EDTDSDTF, MDSTTF, BMDTTTF, Pd(dmit)2, and Ni(dcit)2 By G.C. Papavassiliou, G. Mousdis, V. Kakoussis, A. Terzis, A. Hountas, B. Hilti, C.W. Mayer, and J.S. Zambounis (With 2 Figures) 247

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Part VII Crystal and Electronic Structures

Structural Instabilities and Electronic Structures of Some Organic Conductors and Superconductors By S. Ravy, E. Canadell, and J.P. Pouget (With 5 Figures) 252 Structural and Physical Properties of (BEDT-TTF)2[KHg(SCN)4] By M. Oshima, H. Mori, G. Saito, and K. Oshima (With 9 Figures) . . . . 257 Importance of Weak Hydrogen Bonding C-H-Donor and C-H"Anion Interactions in Governing the Structural Properties of Organic Donors BEDT-TTF and BEDO-TTF and Their Charge-Transfer Salts By M.-H. Whangbo, D. Jung, J. Ren, M. Evain, JJ. Novoa, F. Mota, S. Alvarez, J.M. Williams, M.A. Beno, A.M. Kini, H.H. Wang, and J.R. Ferraro 262 Electronic Structure of /^-(BEDT-TTF)^ Studied by Positron Annihilation By S. Tanigawa, P.K. Tseng, T. Kurihara, K.Y. Chang, K. Watanabe, T. Kubota, M. Tokumoto, N. Kinoshita, and H. Anzai (With 6 Figures) . 267 Pressure Dependence of the Transport Properties of K-(BEDT-TTF)2Cu(NCS)2 By I.D. Parker, R.H. Friend, M. Kurmoo, P. Day, С Lenoir, and P. Batail (With 2 Figures) 272 Anomalous Transport Behavior in K-(BEDT-TTF)2CU(NCS)2

By K. Oshima, R.C. Yu, P.M. Chaikin, H. Urayama, H. Yamochi, and G. Saito (With 2 Figures) 276 STM Study of (BEDT-TTF)2Cu(NCS)2 Surface By M. Yoshimura, N. Ara, M. Kageshima, R. Shioda, A. Kawazu, H. Shigekawa, H. Mori, M. Oshima, H. Yamochi, and G. Saito (With 5 Figures) 280 Crystal Growth and Properties of (BEDT-TTF)2Cu(NCS)2 By Y. Ueba, T. Mishima, H. Kusuhara, and K. Tada (With 4 Figures) . . 284 Synthesis, Crystal Structure and Properties of (BEDT-TTF)3CuCl4H20 By M. Kurmoo, T. Mallah, P. Day, I. Marsden, M. Allan, R.H. Friend, F.L. Pratt, W. Hayes, D. Chasseau, J. Gaultier, and G. Bravic (With 2 Figures) 290 Electronic Properties of Charge Transfer Complexes of BEDT-TTF and Related Donors with Transition Metal Halides By T. Enoki, I. Tomomatsu, Y. Nakano, K. Suzuki, and G. Saito (With 4 Figures) 294 Structural Electrical and Magnetic Properties of the (BEDT-TTF)4Ni(CN)4 Complex By M. Tanaka, H. Takeuchi, A. Kawamoto, J. Tanaka, T. Enoki, K. Suzuki, K. Imaeda, and H. Inokuchi (With 4 Figures) 298

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Crystal Structures and Electrical Conductivities of EDT-TTF Salts with T a F 6 " , A s F 6 " , P F 6 ~ , R e 0 4 " , CIO4-, B F 4 " , Au(CN)2" and Ni(dmit)2"-By A. Kobayashi, R. Kato, and H. Kobayashi (With 2 Figures) 302

A New Transformable Cation-Radical Salt (EPT)2I7 By V.E. Korotkov, R.P. Shibaeva, N.D. Kushch, and E.B. Yagubskii (With 1 Figure) 306

Microwave Conductivity of the Phthalocyanine and Dicyanoquinonediimine Salts By H. Yamakado, A. Ugawa, T. Ida, and K. Yakushi (With 2 Figures) . . 311

Electron-Molecular Vibration Coupling in Organic Superconductors By T. Sugano and M. Kinoshita (With 2 Figures) 315

Dynamics of Charged Domain Walls in Semiconducting Charge Transfer Compounds By Y. Iwasa, N. Watanabe, T. Koda, S. Koshihara, Y. Tokura, N. Iwasawa, and G. Saito (With 4 Figures) 319

The Effect of Pressure on the High Magnetic Field Electronic Phase Transition in Graphite By Y. lye, С Murayama, N. Mori, S. Yomo, J.T. Nicholls, and G. Dresselhaus (With 4 Figures) 324

Ferro- and Antiferromagnetic Intermolecular Interactions of Organic Radicals, a-Nitronyl Nitroxides By K. Awaga, T. Inabe, U. Nagashima, and Y. Maruyama (With 3 Figures) 329

Part VIII Structural Design of Organic Superconductors

Structure-Property Correlations in the Design of Organic Metals and Superconductors: An Overview By A.M. Kini, M.A. Beno, K.D. Carlson, J.R. Ferraro, U. Geiser, AJ . Schultz, H.H. Wang, J.M. Williams, and M.-H. Whangbo (With 4 Figures) 334

Organic Conductors and Superconductors Based on (BEDT-TTF)-Polyiodides By R.P. Shibaeva, E.B. Yagubskii, E.E. Laukhina, and V.N. Laukhin (With 2 Figures) 342

Stoichiometry Control in Organic Metals By K. Bechgaard, K. Lerstrup, M. J0rgensen, I. Johannsen, and J. Christensen (With 8 Figures) 349

Unusual Molecular Systems of Organic-Inorganic Character and Increased Architectural Complexity By P. Batail, K. Boubekeur, A. Davidson, M. Fourmigue, C. Lenoir, C. Livage, and A. Penicaud (With 4 Figures) 353

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Part IX New Molecules and Materials

Salts Derived from Bis(ethylenedioxa)tetrathiafulvalene ("BO") By F. Wudl, H. Yamochi, T. Suzuki, H. Isotalo, С Fite, К. Liou, H. Kasmai, and G. Srdanov (With 7 Figures) 358

New Cation-Radical Salts (ET)3CuCl4 • H20 and (ET)2CuCl4 with Metallic and Semiconducting Properties By A.V. Gudenko, V.B. Ginodman, V.E. Korotkov, A.V. Koshelap, N.D. Kushch, V.N. Laukhin, L.P. Rozenberg, A.G. Khomenko, R.P. Shibaeva, and E.B. Yagubskii (With 5 Figures) 364

New Organic Synthetic Metals Derived from BEDT-TTF, Ni(dsit)2 and BEDO-TTF By M.A. Beno, A.M. Kini, U. Geiser, H.H. Wang, K.D. Carlson, and J.M. Williams (With 3 Figures) 369

Synthesis and Crystal Structures of Multi-Chalcogen TTF Derivatives and Conducting Organic Salts By T. Nogami, H. Nakano, S. Bcegawa, K. Miyawaki, Y. Shirota, S. Harada, and N. Kasai (With 4 Figures) 373

Preparation of Methylated BEDT-TTFs for Controlling Intermolecular S-S Contacts By A. Izuoka, S. Matsumiya, and T. Sugawara (With 3 Figures) 379

Preparation and Properties of Dimeric TTFs By K. Lerstrup, M. j0rgensen, I. Johannsen, and K. Bechgaard (With 1 Figure) 383

Preparation and Properties of p-Quinodimethane Analogues of Tetrathiafulvalene By Y. Yamashita, Y. Kobayashi, and T. Miyashi 387

Syntheses and Physical Properties of Oligothiophene Charge-Transfer Complexes By S. Hotta and K. Waragai (With 4 Figures) 391

3,3':4,4/-Bis(thienot2,3-b]thiophene) with an Isoelectronic Structure of Perylene By T. Otsubo, Y. Kono, H. Miyamoto, Y. Aso, F. Ogura, T. Tanaka, and M. Sawada (With 1 Figure) 395

Design of Organic Molecular Metals Based on New Multi-Stage Redox Systems in the Non-TTF Family: Peri-Condensed Weitz-Type Donors By K. Nakasuji (With 2 Figures) 399

Conjugated Heteroquinonoid Isologues of TCNQ as Novel Electron Acceptors By F. Ogura, K. Yui, H. Ishida, Y. Aso, and T. Otsubo (With 1 Figure) . 403

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Design of Two-Dimensional Stacking Structures: Twin-Type Molecules and Steric Interaction of Axial Substituents By T. Inabe, T. Mitsuhashi, and Y. Maruyama (With 3 Figures) 408

New Molecular Conductors Based on Metal Complex Anions By A.E. Underbill, K.S. Varma, R.A. Clark, and C.E. Wainwright 412

Conducting Evaporated Film of Pt2(CH3CS2)4l By I. Shirotani, Y. Inagaki, and M. Yamashita (With 4 Figures) 416

Electroactive Langmuir Blodgett Films of Tetrathiafulvalene Derivatives By A.S. Dhindsa, M.R. Bryce, and M.C. Petty (With 2 Figures) 420

Physical Properties of Conductive Langmuir-B lodge« Films of Tridecylmethylammonium-Au(dmit)2 and Its Derivatives By T. Nakamura, Y. Miura, M. Matsumoto, H. Tachibana, M. Tanaka, and Y. Kawabata (With 2 Figures) 424

Polymerization of Diacetylenes in Liquid Crystal Phases and Its Application to the Preparation of High Spin Polydiacetylenes By A. Izuoka, T. Okuno, and T. Sugawara (With 3 Figures) 428

Part X Theory

Novel Superconductivity from an Insulator By Y. Takada and M. Kohmoto (With 1 Figure) 434

Bethe Ansatz Wavefunction, Momentum Distribution and Spin Correlation in the One-Dimensional Strongly Correlated Hubbard Model By M. Ogata and H. Shiba (With 4 Figures) 438

New High-Temperature Cooper-Pairing Phase for Vibronic Superconductivity By A. Tachibana, S. Ishikawa, T. Tada, and T. Yamabe (With 4 Figures) 444

Examination of Pairing via Effective van der Waals Interaction in High-Temperature Superconductivity By K. Tanaka, Y. Yamaguchi, and T. Yamabe (With 1 Figure) 449

Reassessment of the Excitonic Mechanism of Little's Superconductivity By K. Tanaka, M. Okada, Y. Huang, and T. Yamabe (With 2 Figures) . . 453

Multi-Valence Resonance-Condensation Model: A Possible Novel and Universal Origin of Superconductivity By A. Nakamura (With 2 Figures) 457

Density Functional Theory for the New High-Temperature Superconducting Phase Transition By A. Tachibana (With 4 Figures) 461

Possible Role of Two-Dimensionality for the Enhancement of Superconducting Tc

By K. Fukushima and H. Sato (With 1 Figure) 465

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Part XI Summary

New Developments That Emerged in the ISSP Symposium By T. Ishiguro 470

Index of Contributors 475

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