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122 Structure and Bonding 122 Structure and Bonding Series Editor: D. M. P.Mingos Editorial Board: P.Day·T.J.Meyer·H.W.Roesky·J.-P.Sauvage Structure and Bonding Series Editor: D. M. P.Mingos Recently Published and Forthcoming Volumes Single-Molecule Magnets Principles and Applications and Related Phenomena of Density Functional Theory Volume Editor: Winpenny, R. in Inorganic Chemistry II Vol. 122, 2006 Volume Editors: Kaltsoyannis, N., McGrady, J. E. Non-Covalent Multi-Porphyrin Assemblies Vol. 113, 2004 Synthesis and Properties Volume Editor: Alessio, E. Principles and Applications Vol. 121, 2006 of Density Functional Theory in Inorganic Chemistry I Recent Developments in Mercury Sience Volume Editors: Volume Editor: Atwood, David A. Kaltsoyannis, N., McGrady, J. E. Vol. 120, 2006 Vol. 112, 2004 Layered Double Hydroxides Supramolecular Assembly Volume Editors: Duan, X., Evans, D. G. via Hydrogen Bonds II Vol. 119, 2005 Volume Editor: Mingos, D. M. P. Vol. 111, 2004 Semiconductor Nanocrystals and Silicate Nanoparticles Applications of Evolutionary Computation Volume Editors: Peng, X., Mingos, D. M. P. in Chemistry Vol. 118, 2005 Volume Editors: Johnston, R. L. Vol. 110, 2004 Magnetic Functions Beyond the Spin-Hamiltonian Fullerene-Based Materials Volume Editor: Mingos, D. M. P. Structures and Properties Vol. 117, 2005 Volume Editor: Prassides, K. Vol. 109, 2004 Intermolecular Forces and Clusters II VolumeEditor:Wales,D.J. Supramolecular Assembly Vol. 116, 2005 via Hydrogen Bonds I Volume Editor: Mingos, D. M. P. Intermolecular Forces and Clusters I Vol. 108, 2004 VolumeEditor:Wales,D.J. Vol. 115, 2005 Optical Spectra and Chemical Bonding in Transition Metal Complexes Superconductivity in Complex Systems Special Volume II Volume Editor: Müller, K. A. dedicated to Professor Jørgensen Vol. 114, 2005 Volume Editor: Schönherr, T. Vol. 107, 2004 Single-Molecule Magnets and Related Phenomena Volume Editor: Richard Winpenny With contributions by G. Aromí · B. Barbara · E. K. Brechin · A. Caneschi R. Clérac · A. Cornia · A. F. Costantino · C. Coulon J. Curély · D. Gatteschi · T. Mallah · M. Mannini E. J. L. McInnes · H. Miyasaka · J.-N. Rebilly R. Sessoli · L. Zobbi 123 The series Structure and Bonding publishes critical reviews on topics of research concerned with chemical structure and bonding. The scope of the series spans the entire Periodic Table. It focuses attention on new and developing areas of modern structural and theoretical chemistry such as na- nostructures, molecular electronics, designed molecular solids, surfaces, metal clusters and supra- molecular structures. Physical and spectroscopic techniques used to determine, examine and model structures fall within the purview of Structure and Bonding to the extent that the focus is on the scientific results obtained and not on specialist information concerning the techniques themselves. Issues associated with the development of bonding models and generalizations that illuminate the reactivity pathways and rates of chemical processes are also relevant. As a rule, contributions are specially commissioned. The editors and publishers will, however, always be pleased to receive suggestions and supplementary information. Papers are accepted for Structure and Bonding in English. In references Structure and Bonding is abbeviated Struct Bond and is cited as a journal. Springer WWW home page: springer.com Visit the Struct Bond content at springerlink.com Library of Congress Control Number: 2006926433 ISSN 0081-5993 ISBN-10 3-540-33239-1 Springer Berlin Heidelberg New York ISBN-13 978-3-540-33239-8 Springer Berlin Heidelberg New York DOI 10.1007/b104234 This work is subject to copyright. All rights are reserved, whether the whole or part of the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation, broad- casting, reproduction on microfilm or in any other way, and storage in data banks. Duplication of this publication or parts thereof is permitted only under the provisions of the German Copyright Law of September 9, 1965, in its current version, and permission for use must always be obtained from Springer. Violations are liable for prosecution under the German Copyright Law. Springer is a part of Springer Science+Business Media springer.com c Springer-Verlag Berlin Heidelberg 2006 Printed in Germany The use of registered names, trademarks, etc. in this publication does not imply, even in the absence of a specific statement, that such names are exempt from the relevant protective laws and regulations and therefore free for general use. Cover design: Design & Production GmbH, Heidelberg Typesetting and Production: LE-TEXJelonek,Schmidt&VöcklerGbR,Leipzig Printed on acid-free paper 02/3100 YL – 5 4 3 2 1 0 Series Editor Prof. D. Michael P. Mingos Principal St. Edmund Hall Oxford OX1 4AR, UK [email protected] Volume Editor Prof. Richard Winpenny Department of Chemistry The University of Manchester Oxford Road Manchester M13 9PL, UK [email protected] Editorial Board Prof. Peter Day Prof. Herbert W. Roesky Director and Fullerian Professor Institut for Anorganic Chemistry of Chemistry University of Göttingen The Royal Institution of Great Britain Tammannstr. 4 21 Albermarle Street 37077 Göttingen, Germany London W1X 4BS, UK [email protected] [email protected] Prof. Jean-Pierre Sauvage Prof. Thomas J. Meyer Faculté de Chimie Department of Chemistry Laboratoires de Chimie Campus Box 3290 Organo-Minérale Venable and Kenan Laboratories Université Louis Pasteur The University of North Carolina 4, rue Blaise Pascal and Chapel Hill 67070 Strasbourg Cedex, France Chapel Hill, NC 27599-3290, USA [email protected] [email protected] Structure and Bonding Also Available Electronically For all customers who have a standing order to Structure and Bonding, we offer the electronic version via SpringerLink free of charge. Please contact your librarian who can receive a password or free access to the full articles by registering at: springerlink.com If you do not have a subscription, you can still view the tables of contents of the volumes and the abstract of each article by going to the SpringerLink Home- page, clicking on “Browse by Online Libraries”, then “Chemical Sciences”, and finally choose Structure and Bonding. You will find information about the – Editorial Board –AimsandScope – Instructions for Authors –SampleContribution at springer.com using the search function. Preface In some ways the story of single-molecule magnets (SMMs) starts with work performed in the Christou group during the 1980s. The research was dedi- cated to the synthesis of model compounds of the oxygen-evolving complex in Photosystem II. The work resulted in a very large number of polymetallic mixed-valent manganese complexes being made—many having rather more metal centres than are strictly speaking required for an accurate representation oftheactivesiteoftheenzyme. The work had produced many beautiful model compounds and was very well reviewed at the time [1], but lacked a model for the highest oxidation state of the biological cycle. In attempting to make such a model by oxi- dation of manganese acetate with permanganate, a compound of formula [Mn12O12(O2CPh)16(H2O)4] was isolated [2]. This was a new compound, but rather surprisingly it had a very close precedent: in 1980 Lis had made [Mn12O12(O2CMe)16(H2O)4] and published the crystal structure [3]. Lis also included preliminary magnetic measurements from 4–300 K, but did not in- terpret them. Even more surprisingly the first proposal of a dodecanuclear manganese complex from this type of reaction was made in 1921 by Weinland and Fischer [4], although given the equipment available at the time Wein- land and Fischer did not get the metal-to-ligand stoichiometry correct. The rediscovery by the Christou group was therefore serendipitous. Boydet al. measuredthemagnetic propertiesof [Mn12O12(O2CPh)16(H2O)4] and deduced a spin ground state of S =14[2].Thisisincorrect,butthemis- take is unsurprising in that the behaviour of this compound is unlike that of previously prepared high-spin molecules. At that time, the highest spin known for a molecule was S = 12, for a molecule reported by Gatteschi’s group [5]. As a result of the paper by Boyd et al. the Gatteschi group reinvestigated the Lis compound by high-field magnetisation and high-frequency EPR spectroscopy. The resulting paper, published by Caneschi et al. in 1991 [6], describes the freez- ing of the magnetisation at low fields, and also explains this behaviour—which is analogous to that of superparamagnets—due to the negative axial anisotropy of the high-spin ground state of the compound. The ground state was found to be S = 10, and later measurements show that [Mn12O12(O2CPh)16(H2O)4] also has an S = 10 ground state [7, 8]. The paper by Caneschi et al. [6] misses one trick: the term single-molecule magnet is not used, however this is now X Preface how these molecules are universally known. Despite the lack of a snappy title this paper introduces many of the basic ideas underlying the physics of SMMs. These initial discoveries have provided physicists with ideal objects for studying quantum phenomena, such as tunnelling of magnetisation. This was first reported by Barbara and co-workers [9], and simultaneously by Friedman et al. [10]. Many following studies have been designed to understand these phenomena and the mechanism of tunnelling. The advantage in studying the physics of SMMs over particulate supraparamagnets is that coordination chemists can vary the physical properties of the quantum objects using the skills of a synthetic chemist. The result has been a remarkably large number of derivatives of “Mn12”. Reviews of the physics and the quantum phenomena of SMMs have been published previously [11, 12], therefore here we have concentrated on aspects that have not been reviewed. Aromi and Brechin explore synthetic routes to SMMs, covering the literature exhaustively until May 2005. McInnes has reviewed the spectroscopic studies of SMMs published until mid-2005. Mallah has reviewed the use of metallocyanates in making SMMs, and Cornia has reviewed the growing field of hybrid materials featuring SMMs.
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