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Magnetism, Molecule-Based Materials (Magnetism: Molecules to Materials):

[size=120%]Magnetism , Molecule-Based Materials (Magnetism: Molecules to Materials)
By Joel S. Miller, Marc Drillon

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Binding: Hardcover

Product Description:
Molecule-based magnets, giant magnetoresistance and spin frustration are just a few terms which demonstrate that our understanding of magnetic behavior, once thought to be mature, has enjoyed new momentum as it is being expanded by contributions from molecular chemistry, materials chemistry and sciences to solid state physics. The spectrum spans molecule-based - organic, inorganic, and hybrid - compounds, metallic materials as well as their oxides forming thin films, nanoparticles, wires etc. New phenomena are explored that open promising perspectives for commercially applied "smart" materials.
In topical reviews written by foremost scientists trends and recent advances focusing on the correlations between electronic structure and magnetic properties are explained in a clear and detailed way. With good balance between theory and experiment this book guides advanced students and specialists alike to this research area. It facilitates the evaluation of experimental observations and serves as a base for the design of new magnetic materials. As a unique reference work, it is indispensable for everyone concerned with the phenomena of magnetism!

Contents
1 Nitroxide-based Organic Magnets . . . . . . . . . . . . . . . . . . . . . . 1
1.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.2 Unconjugated Nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . 5
1.2.1 Mono-nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . 5
1.2.2 Oligo-nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . . 10
1.3 Conjugated Nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . . 12
1.3.1 Mono-nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . 12
1.3.2 Oligo-nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . . 14
1.4 Nitronyl Nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
1.4.1 Mono-nitronyl Nitroxides . . . . . . . . . . . . . . . . . . . . 18
1.4.2 Oligo-nitronyl Nitroxides . . . . . . . . . . . . . . . . . . . . 35
1.4.3 Co-crystallization of Nitronyl Nitroxides . . . . . . . . . . . . 40
1.5 Imino Nitroxides . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 44
1.6 Poly(nitroxides) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46
1.7 Outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 49
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 51
2 Magnetic Ordering in Metal Coordination Complexes
with Aminoxyl Radicals . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
2.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
2.2 Aminoxyl Radicals . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
2.2.1 Electronic Structure and Basicity . . . . . . . . . . . . . . . . 62
2.2.2 Aminoxyl Radicals with Another Basic Center . . . . . . . . 63
2.2.3 High-spin Di- and Poly(aminoxyl) Radicals . . . . . . . . . . 64
2.3 Magnetic Interaction between Transition Metal Ions
and Aminoxyl Radicals . . . . . . . . . . . . . . . . . . . . . . . . . . 65
2.3.1 Indirect Coupling (Extended Superexchange) . . . . . . . . . 65
2.3.2 Complexes with Direct Metal-Aminoxyl Coordination . . . . 70
2.3.3 Cyclic Complexes . . . . . . . . . . . . . . . . . . . . . . . . . 72
2.4 Design Strategy for Various Crystyl Structures . . . . . . . . . . . . . 74
2.5 Preparation of 3d Transition Metal-Poly(aminoxyl)
Radical Complexes . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77
2.6 One-dimensional Metal-Aminoxyl Systems . . . . . . . . . . . . . . 80
2.6.1 Structure and Magnetic Properties of Ferrimagnetic
1D Chains Formed by Manganese(II) and
Nitronyl Nitroxides . . . . . . . . . . . . . . . . . . . . . . . . 81
Magnetism: Molecules to Materials II: Molecule-Based Materials.
Edited by Joel S. Miller and Marc Drillon
Copyright c 2002Wiley-VCH Verlag GmbH & Co. KGaA
ISBNs: 3-527-30301-4 (Hardback); 3-527-60059-0 (Electronic)
VI Contents
2.6.2 Structure and Magnetic Properties of Ferrimagnetic
1D Chains Formed by Manganese(II) and
Triplet bis-Aminoxyl Radicals . . . . . . . . . . . . . . . . . . 82
2.7 Two-dimensional Metal-Aminoxyl Systems . . . . . . . . . . . . . . . 88
2.7.1 Structure and Magnetic Properties of Ferrimagnetic
2D Sheets Formed by Manganese(II) and
Nitronyl Nitroxides . . . . . . . . . . . . . . . . . . . . . . . . 89
2.7.2 Structure and Magnetic Properties of Ferrimagnetic
2D Sheets Formed by Manganese(II) and
High-spin tris-Aminoxyl Radicals . . . . . . . . . . . . . . . . 90
2.7.3 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 97
2.8 Three-dimensional Metal-Aminoxyl Systems . . . . . . . . . . . . . . 97
2.8.1 Crystal and Molecular Structure of the 3D System . . . . . . 98
2.8.2 Magnetic Properties of the 3D System . . . . . . . . . . . . . 99
2.8.3 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 104
2.9 Summary and Prognosis . . . . . . . . . . . . . . . . . . . . . . . . . 104
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 105
3 Organic Kagome Antiferromagnets . . . . . . . . . . . . . . . . . . . . . . 109
3.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 109
3.2 Inorganic Kagome Antiferromagnets . . . . . . . . . . . . . . . . . . 110
3.2.1 SrGa12-xCrxO19 (SCGO(x)) . . . . . . . . . . . . . . . . . . . 110
3.2.2 Jarosite, AM3(OH)6(SO4)2 (A = Na+, K+, Rb+, Ag+, NH+4,
H3O+, etc., and M = Fe3+ or Cr3+) . . . . . . . . . . . . . . . 111
3.3 Organic Kagome Antiferromagnet, m-MPYNN·X . . . . . . . . . . 111
3.3.1 Crystal Structure . . . . . . . . . . . . . . . . . . . . . . . . . 111
3.3.2 Magnetic Susceptibility . . . . . . . . . . . . . . . . . . . . . . 113
3.3.3 Heat Capacity . . . . . . . . . . . . . . . . . . . . . . . . . . . 115
3.3.4 Positive Muon Spin Rotation . . . . . . . . . . . . . . . . . . 116
3.3.5 Distorted Kagome Lattices . . . . . . . . . . . . . . . . . . . . 117
3.3.6 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 120
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 120
4 Magnetism in TDAE-C60 . . . . . . . . . . . . . . . . . . . . . . . . . . . 123
4.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 123
4.2 Synthesis and Structure . . . . . . . . . . . . . . . . . . . . . . . . . . 124
4.2.1 Synthesis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 124
4.2.2 The Lattice Structure . . . . . . . . . . . . . . . . . . . . . . . 126
4.3 The Electronic Structure . . . . . . . . . . . . . . . . . . . . . . . . . 128
4.4 The Magnetic Properties . . . . . . . . . . . . . . . . . . . . . . . . . 130
4.4.1 The Bulk Magnetic Properties . . . . . . . . . . . . . . . . . . 130
4.4.2 The Spin-glass Behavior of α -TDAE-C60 . . . . . . . . . . . 134
4.4.3 Electron-spin Resonance . . . . . . . . . . . . . . . . . . . . . 135
4.4.4 Ferromagnetic Resonance . . . . . . . . . . . . . . . . . . . . 137
4.5 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 144
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 145
Contents VII
5 Triarylmethyl and Amine Radicals . . . . . . . . . . . . . . . . . . . . . . 149
5.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 149
5.2 Monoradicals (S = 1/2) . . . . . . . . . . . . . . . . . . . . . . . . . . 149
5.3 Diradicals (S=1) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 153
5.4 Triradicals (S = 3/2) . . . . . . . . . . . . . . . . . . . . . . . . . . . . 161
5.5 Monodisperse High-spin Oligomers (S=2–ca. 10) . . . . . . . . . . 163
5.6 High-spin Polymers (up to Sn =ca. 48) . . . . . . . . . . . . . . . . . 179
5.7 Conclusions and Prospects (Beyond S = ca. 48?) . . . . . . . . . . . . 182
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 185
6 High-spin Metal-ion-containing Molecules . . . . . . . . . . . . . . . . . . 189
6.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 189
6.2 Self-assembly of Molecular Clusters . . . . . . . . . . . . . . . . . . . 190
6.2.1 Competing Interactions and Spin Frustration . . . . . . . . . 190
6.2.2 The Carboxylate Family . . . . . . . . . . . . . . . . . . . . . 192
6.2.3 The Hydroxypyridonate Family . . . . . . . . . . . . . . . . . 197
6.3 Host-Guest Approach . . . . . . . . . . . . . . . . . . . . . . . . . . 201
6.3.1 Hexanuclear Iron(III) Rings . . . . . . . . . . . . . . . . . . . 202
6.3.2 Hexanuclear Manganese Rings . . . . . . . . . . . . . . . . . 203
6.4 Step-by-step Rationale Approach . . . . . . . . . . . . . . . . . . . . 204
6.4.1 Complex as Ligand and Complex as Metal . . . . . . . . . . . 206
6.4.2 Predicting the Spin Ground State . . . . . . . . . . . . . . . . 207
6.4.3 Antiferromagnetic Approach . . . . . . . . . . . . . . . . . . 208
6.4.4 Ferromagnetic Approach . . . . . . . . . . . . . . . . . . . . . 211
6.4.5 Role of the Organic Ligand . . . . . . . . . . . . . . . . . . . 214
6.4.6 Molecules with Two Shells of Paramagnetic Species . . . . . 217
6.5 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 223
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 223
7 Electronic Structure and Magnetic Behavior
in Polynuclear Transition-metal Compounds . . . . . . . . . . . . . . . . . 227
7.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 227
7.2 Phenomenological Description of Exchange Coupling:
the Heisenberg Hamiltonian . . . . . . . . . . . . . . . . . . . . . . . 228
7.3 Qualitative Models of the Exchange Coupling Mechanism . . . . . . 230
7.3.1 Orthogonal Magnetic Orbitals . . . . . . . . . . . . . . . . . . 230
7.3.2 Natural Magnetic Orbitals . . . . . . . . . . . . . . . . . . . . 234
7.4 Quantitative Evaluation of Exchange Coupling Constants . . . . . . 235
7.4.1 Perturbative and Variational Calculations
of State Energy Differences . . . . . . . . . . . . . . . . . . . 236
7.4.2 Ab initio Calculations of State Energies . . . . . . . . . . . . 240
7.4.3 Calculations using Broken-symmetry Functions . . . . . . . . 242
7.5 Exchange Coupling in Polynuclear Transition-metal Complexes . . . 249
7.5.1 Homodinuclear Compounds . . . . . . . . . . . . . . . . . . . 249
7.5.2 Heterodinuclear Compounds . . . . . . . . . . . . . . . . . . 261
VIII Contents
7.5.3 Polynuclear Compounds . . . . . . . . . . . . . . . . . . . . . 263
7.5.4 Solid-state Compounds: The Case of Cu2(OH)3NO3 . . . . . 266
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 271
8 Valence Tautomerism in Dioxolene Complexes of Cobalt . . . . . . . . . 281
8.1 Introduction – Bistability, Hysteresis,
and Electronically Labile Materials . . . . . . . . . . . . . . . . . . . 281
8.1.1 Bistability and Hysteresis . . . . . . . . . . . . . . . . . . . . 281
8.1.2 Electronically Labile Materials . . . . . . . . . . . . . . . . . 281
8.2 Valence Tautomerism in Dioxolene Complexes of Cobalt . . . . . . 284
8.2.1 Valence Tautomerism – A General Chemical Description . . 284
8.2.2 Valence Tautomerism – A Simplified MO Description . . . . 287
8.2.3 VT Thermodynamics . . . . . . . . . . . . . . . . . . . . . . . 288
8.2.4 Experimental Determination of Thermodynamic Parameters 290
8.2.5 Dependence of KVT Equilibrium on Ancillary Ligands . . . 292
8.2.6 Pressure-induced VT . . . . . . . . . . . . . . . . . . . . . . . 297
8.2.7 Light-induced VT and Rates of VT . . . . . . . . . . . . . . . 299
8.2.8 VT Complexes of Other Quinone Ligands
and Redox Chemistry of VT Complexes . . . . . . . . . . . . 300
8.2.9 Polymeric VT Materials . . . . . . . . . . . . . . . . . . . . . 302
8.3 Future Directions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 303
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
9 Molecule-based Magnets Derived from NiII and MnII
Azido Bridging Ligand and Related Compounds . . . . . . . . . . . . . . 307
9.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
9.2 Synthetic Procedures . . . . . . . . . . . . . . . . . . . . . . . . . . . 308
9.3 Exchange-coupling Parameter . . . . . . . . . . . . . . . . . . . . . . 309
9.4 Molecular-based Magnetic Materials . . . . . . . . . . . . . . . . . . 309
9.5 One-dimensional Systems . . . . . . . . . . . . . . . . . . . . . . . . 312
9.5.1 With 1,3-Azido Bridging Ligands (AF, Uniform) . . . . . . . 312
9.5.2 With 1,3-Azido Bridging Ligands (AF, Alternating) . . . . . 313
9.5.3 With 1,1-Azido Bridging Ligands (Ferromagnetic) . . . . . . 316
9.5.4 With 1,3-N3 and 1,1-N3 bridges . . . . . . . . . . . . . . . . . 319
9.6 Two-dimensional Systems . . . . . . . . . . . . . . . . . . . . . . . . . 322
9.6.1 With Only Azido as Bridging Ligand . . . . . . . . . . . . . . 322
9.7 Three-dimensional Systems . . . . . . . . . . . . . . . . . . . . . . . . 329
9.8 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 334
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 335
10 Oxalate-based 2D and 3D Magnets . . . . . . . . . . . . . . . . . . . . . . 339
10.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 339
10.2 Basic Principles of Specific 2D and 3D Network Configurations . . . 339
10.3 Structural Studies on 2D Oxalato Bridged Compounds . . . . . . . . 344
10.4 Magnetic Studies on 2D Oxalato Bridged Compounds . . . . . . . . 346
10.5 Structural Studies on 3D Oxalato Bridged Compounds . . . . . . . . 349
Contents IX
10.6 Magnetic Studies on 3D Oxalato Bridged Compounds . . . . . . . . 352
10.7 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 354
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 355
11 Hybrid Organic-Inorganic Multilayer Compounds:
Towards Controllable and/or Switchable Magnets . . . . . . . . . . . . . . 357
11.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 357
11.2 Hydroxide-based Layered Compounds . . . . . . . . . . . . . . . . . 358
11.3 Anion-exchange Reactions . . . . . . . . . . . . . . . . . . . . . . . . 360
11.4 Influence of Organic Spacers in Hydroxide-based Compounds . . . . 361
11.4.1 The Cu2(OH)3X Series . . . . . . . . . . . . . . . . . . . . . . 361
11.4.2 The Co2(OH)3X Series . . . . . . . . . . . . . . . . . . . . . . 364
11.4.3 Dipolar Interaction and Long-range Magnetic Order . . . . . 367
11.5 Difunctional Organic Anions Connecting Magnetic Layers . . . . . . 370
11.6 Metal-radical-based Layered Magnets . . . . . . . . . . . . . . . . . 376
11.7 Controllable Magnetic Properties of Layered Copper Hydroxides . . 380
11.7.1 Solvent-mediated Magnetism . . . . . . . . . . . . . . . . . . 380
11.7.2 Photoisomerism of Azobenzenes
in Layered Copper Hydroxides . . . . . . . . . . . . . . . . . 384
11.8 Layered Perovskite Ferromagnets . . . . . . . . . . . . . . . . . . . . 385
11.8.1 High-pressure Effects . . . . . . . . . . . . . . . . . . . . . . . 386
11.8.2 Spontaneous Magnetization
in Layered Perovskite Ferromagnets . . . . . . . . . . . . . . 389
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 393
12 Intercalation-induced Magnetization
in MPS3 Layered Compounds . . . . . . . . . . . . . . . . . . . . . . . . . 397
12.1 Introduction and Scope . . . . . . . . . . . . . . . . . . . . . . . . . . 397
12.2 Structural and Electronic Aspects . . . . . . . . . . . . . . . . . . . . 397
12.3 Magnetic Properties of the Pristine MPS3 Phases (M = Mn, Fe, Ni) . 399
12.4 Ion-exchange Intercalation into the MPS3 Compounds . . . . . . . . 401
12.5 The Magnetic Properties of the MnPS3 Intercalates . . . . . . . . . . 402
12.5.1 General . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 402
12.5.2 X-ray and Neutron-diffraction Study
of Selected Intercalates . . . . . . . . . . . . . . . . . . . . . . 405
12.5.3 A Ferrimagnetic Model of the MnPS3 Intercalates:
Imbalancing of Spins . . . . . . . . . . . . . . . . . . . . . . . 407
12.6 The Magnetic Properties of the FePS3 Intercalates . . . . . . . . . . 410
12.6.1 General . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 410
12.6.2 Spectroscopic Characterization of the FePS3 Intercalates . . 413
12.6.3 Discussion on the Role of Intercalation into FePS3 . . . . . . 415
12.6.4 Magnetic Properties of Iron-diluted
Fe1−xCdxPS3 Compounds . . . . . . . . . . . . . . . . . . . . 416
12.6.5 Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 417
12.7 The NiPS3-Cobaltocene Intercalation Compound . . . . . . . . . . . 419
X Contents
12.8 Multi-property Materials:
Associating Magnetism and Non-linear Optics . . . . . . . . . . . . . 420
12.9 Conclusion and Perspectives . . . . . . . . . . . . . . . . . . . . . . . 421
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 421
13 Transition Metal Ion Phosphonates
as Hybrid Organic–Inorganic Magnets . . . . . . . . . . . . . . . . . . . . 425
13.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 425
13.2 Synthesis of the Ligands . . . . . . . . . . . . . . . . . . . . . . . . . 426
13.3 Vanadium Phosphonates . . . . . . . . . . . . . . . . . . . . . . . . . 426
13.3.1 Preparation . . . . . . . . . . . . . . . . . . . . . . . . . . . . 426
13.3.2 Crystal Structures . . . . . . . . . . . . . . . . . . . . . . . . . 427
13.3.3 Magnetic Properties . . . . . . . . . . . . . . . . . . . . . . . 427
13.4 Divalent Metal Phosphonates . . . . . . . . . . . . . . . . . . . . . . 430
13.4.1 Synthesis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 430
13.4.2 Crystal Structures . . . . . . . . . . . . . . . . . . . . . . . . . 432
13.4.3 Magnetic Properties . . . . . . . . . . . . . . . . . . . . . . . 437
13.5 Metal(II) Diphosphonates . . . . . . . . . . . . . . . . . . . . . . . . 449
13.5.1 Synthesis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 449
13.5.2 Crystal Structures . . . . . . . . . . . . . . . . . . . . . . . . . 450
13.5.3 Magnetic Properties . . . . . . . . . . . . . . . . . . . . . . . 452
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 454
14 Magnetic Langmuir-Blodgett Films . . . . . . . . . . . . . . . . . . . . . . 457
14.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 457
14.2 The Langmuir–Blodgett Technique . . . . . . . . . . . . . . . . . . . 459
14.2.1 Fabrication of Langmuir–Blodgett Films . . . . . . . . . . . . 459
14.2.2 Structural and Physical Characterization
of Langmuir and LB Films . . . . . . . . . . . . . . . . . . . . 461
14.3 Magnetic Systems: A Molecular Approach . . . . . . . . . . . . . . . 462
14.3.1 Hybrid LB Films with Magnetic Clusters . . . . . . . . . . . . 462
14.3.2 Spin-transition Systems . . . . . . . . . . . . . . . . . . . . . . 465
14.3.3 Comments on Molecular Magnetism in LB Films . . . . . . . 468
14.4 Extended Systems and Cooperative Effects . . . . . . . . . . . . . . 469
14.4.1 “Literally Two-Dimensional Magnets” . . . . . . . . . . . . . 469
14.4.2 Metal Phosphonate LB Films . . . . . . . . . . . . . . . . . . 470
14.4.3 Organic and Inorganic “Dual Network” Films . . . . . . . . . 473
14.4.4 Bimetallic Compounds . . . . . . . . . . . . . . . . . . . . . . 475
14.5 Comparison with Other Lamellar and Colloidal Systems . . . . . . . 478
14.5.1 Hybrid Lamellar Systems . . . . . . . . . . . . . . . . . . . . 479
14.5.2 Self-organized Media . . . . . . . . . . . . . . . . . . . . . . . 480
14.6 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 481
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 482
Index . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 485

Magnetism, Molecule-Based Materials (2001).part1