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Topics in Organometallic Chemistry 64 Vadapalli Chandrasekhar Fabrice Pointillart Editors Organometallic Magnets 64 Topics in Organometallic Chemistry Series Editors M. Beller, Rostock, Germany P. H. Dixneuf, Rennes, France J. Dupont, Porto Alegre, Brazil A. Fürstner, Mülheim, Germany F. Glorius, Münster, Germany L. J. Gooßen, Kaiserslautern, Germany S. P. Nolan, Ghent, Belgium J. Okuda, Aachen, Germany L. A. Oro, Zaragoza, Spain M. Willis, Oxford, United Kingdom Q.-L. Zhou, Tianjin, China Aims and Scope The series Topics in Organometallic Chemistry presents critical overviews of researchresultsinorganometallicchemistry.Asourunderstandingoforganometal- lic structure, properties and mechanisms increases, new ways are opened for the design of organometallic compounds and reactions tailored to the needs of such diverseareasasorganicsynthesis,medicalresearch,biologyandmaterialsscience. Thus the scope of coverage includes a broad range of topics of pure and applied organometallic chemistry,wherenew breakthroughs arebeingachievedthat areof significancetoalargerscientificaudience. The individual volumes of Topics in Organometallic Chemistry are thematic. Reviewarticlesaregenerallyinvitedbythevolumeeditors.AllchaptersfromTopics inOrganometallicChemistryarepublishedOnlineFirstwithanindividualDOI.In references, Topics in Organometallic Chemistry is abbreviated as Top Organomet Chemandcitedasajournal. Moreinformationaboutthisseriesathttp://www.springer.com/series/3418 (cid:129) Vadapalli Chandrasekhar Fabrice Pointillart Editors Organometallic Magnets With contributions by (cid:1) (cid:1) (cid:1) (cid:1) J. Autschbach H. Bolvin O. Cador V. Chandrasekhar (cid:1) (cid:1) (cid:1) (cid:1) (cid:1) E. Colacio A. Dey S. Gao F. Gendron T. Gupta (cid:1) (cid:1) (cid:1) (cid:1) M. J. Heras Ojea S.-D. Jiang P. Kögerler T. Korzeniak (cid:1) (cid:1) (cid:1) R. A. Layfield L. C. H. Maddock R. S. Narayanan (cid:1) (cid:1) (cid:1) B. Nowicka F. Pointillart G. Rajaraman (cid:1) (cid:1) (cid:1) M. Shanmugam B. Sieklucka M. K. Singh (cid:1) (cid:1) (cid:1) (cid:1) M. Speldrich J. Tang S. Tripathi J. van Leusen (cid:1) B.-W. Wang Z. Zhu Editors VadapalliChandrasekhar FabricePointillart DepartmentofChemistry InstitutdesSciencesChimiquesdeRennes IndianInstituteofTechnology EquipeOrganométalliques:Matériauxet Kanpur,India Catalyse RennesCedex,France ISSN1436-6002 ISSN1616-8534 (electronic) TopicsinOrganometallicChemistry ISBN978-3-030-26008-8 ISBN978-3-030-26009-5 (eBook) https://doi.org/10.1007/978-3-030-26009-5 ©SpringerNatureSwitzerlandAG2019 Thisworkissubjecttocopyright.AllrightsarereservedbythePublisher,whetherthewholeorpartofthe materialisconcerned,specificallytherightsoftranslation,reprinting,reuseofillustrations,recitation, broadcasting,reproductiononmicrofilmsorinanyotherphysicalway,andtransmissionorinformation storageandretrieval,electronicadaptation,computersoftware,orbysimilarordissimilarmethodology nowknownorhereafterdeveloped. Theuseofgeneraldescriptivenames,registerednames,trademarks,servicemarks,etc.inthispublication doesnotimply,evenintheabsenceofaspecificstatement,thatsuchnamesareexemptfromtherelevant protectivelawsandregulationsandthereforefreeforgeneraluse. The publisher, the authors, and the editorsare safeto assume that the adviceand informationin this bookarebelievedtobetrueandaccurateatthedateofpublication.Neitherthepublishernortheauthorsor theeditorsgiveawarranty,expressedorimplied,withrespecttothematerialcontainedhereinorforany errorsoromissionsthatmayhavebeenmade.Thepublisherremainsneutralwithregardtojurisdictional claimsinpublishedmapsandinstitutionalaffiliations. ThisSpringerimprintispublishedbytheregisteredcompanySpringerNatureSwitzerlandAG. Theregisteredcompanyaddressis:Gewerbestrasse11,6330Cham,Switzerland Preface The discovery, in the 1990s, that the polynuclear mixed valent complex [Mn O (OAc) (H O) ] was a single-molecule magnet (SMM) created a new 12 12 16 2 4 interdisciplinaryfieldinthearea ofmolecularmagnets.Contributionsandcollabo- rationsfromchemists,physicists,andmaterialsscientistsandbetweentheoristsand experimentalistsareallowingthisfieldtogrowvigorously,beingmotivatedbynot only academic questions but also potential applications in high density storage, quantumcomputing,andspintronicdevices.Thesejointeffortshaveledtotheuse of 4f lanthanide ions and the discovery of the first mononuclear complex of TbIII which behaves as an SMM in 2003. Researchers also developed strategies to combine the advantages of both 3d and 4f elements in designing heterobimetallic compounds.Morerecentlythisisbeingextendedtosystemscontaining4d/5dand5f actinideions.Now,morethaneverbefore,molecularmagnetsareintheraceforhigh densitystorageapplicationssincetheirdesignusesorganometallicchemistryandthe observationofmagneticmemoryupto80K. This book aims to illustrate different strategies to design molecular magnets throughtherecentachievementsofthecontributorsandhowbrainstormingbetween experimentalchemists,theoreticiansaswellasphysicistsincreasedtheunderstand- ingandperformanceofthemolecularmagnets.Todoso,thisvolumeisdividedinto eleven chapters. In the chapter “Hybrid Organic-Inorganic Cyanide-Bridged Net- works,” Korzeniak, Nowicka, and Sieklucka reveal strategies to design hybrid organic-inorganic cyanide-bridged networks as molecular magnets. In the chapter “Cobalt(II) Complexes as Single-Ion Magnets”, Tripathi, Dey, Shanmugam, Narayanan, and Chandrasekhar present recent achievements about Co(II) single- ion magnets and in the chapter “Cobalt(II)/(III)–Lanthanide(III) Complexes as Molecular Magnets”, the same authors show how Co(II) can be associated with 4f ionstoobserveslowmagneticrelaxation.Inthechapter“MannichBaseLigandsas VersatilePlatformsforSMMs”,ColaciohighlightstheusefulnessofMannich-base ligandstoassemblehomometallic4fcomplexesandheterometallic3d/4fcomplexes as SMMs. Utility of a specific ligand, viz. the tetrathiafulvalene-based ligand, is showninthechapter“Tetrathiafulvalene-BasedMagnetsofLanthanides”byCador v vi Preface andPointillarttorationallydesignandassemblemono-andpolynuclearSMMs.In thechapter“GeometryandMagnetismofLanthanideCompounds”,Zhu andTang demonstratetheimportanceofthecoordinationgeometriesonthemagneticbehav- ior. In the chapter “Single-Ion Anisotropy: An Insight to Complicated Magnetic Molecules”, Gao, Jiang, and Wang overviewed the theoretical and experimental considerations in constructing mononuclear SMM. Organometallic approach is treated in the chapter “Lanthanide Organometallics as Single-Molecule Magnets” by Ojea, Maddock, and Layfield as a powerful tool toachieve magnetic bistability aboveliquid-nitrogentemperatures.Inthechapter“RoleofAbInitioCalculationsin the Design and Development of Lanthanide Based Single Molecule Magnets”, Gupta,Singh,andRajaramanhighlightthecrucialroleoftheabinitioapproachin theunderstandingofthemagneticpropertiesandthedevelopmentoffuturecoordi- nation and organometallic molecular magnets while the chapter “Complete Active SpaceWavefunction-BasedAnalysisofMagnetizationandElectronicStructure”by Autschbach, Bolvin, and Gendron addresses the complete Active Space Wavefunction-Based Analysis of Magnetization and Electronic Structure for the entire transition metals, lanthanides, and actinides. Finally in the chapter “Magne tismofActinideCoordinationCompounds”,Leusen,Speldrich,andKögerlerintro- duce a model focused on the interpretation of the magnetic properties of a recent classofcoordinationcomplexesinvolvingactinides. Theeditorshopethatthereaderwillbeconvincedaboutthefastprogressinthe understanding of the magnetic properties of molecular magnets thanks to the col- laborative work between experimental researchers (chemists, spectroscopists, and physicists) and theoreticians. Obviously the challenges that remain are still huge including minimizing fast magnetic relaxation (mainly through quantum effects), graftingofmostpromisingsystemsonsurfaceswithoutalterationoftheproperties, andaddressingpropertiesfromsuchsystems. The editors are extremely thankful to all the authors for their contributions to thisbook. Contents HybridOrganic–InorganicCyanide-BridgedNetworks. . . . . . . . . . . . . 1 TomaszKorzeniak,BeataNowicka,andBarbaraSieklucka Cobalt(II)ComplexesasSingle-IonMagnets. . . . . . . . . . . . . . . . . . . . . 35 ShaliniTripathi,AtanuDey,MaheswaranShanmugam, RamakirushnanSuriyaNarayanan,andVadapalliChandrasekhar Cobalt(II)/(III)–Lanthanide(III)ComplexesasMolecularMagnets. . . . 77 AtanuDey,ShaliniTripathi,MaheswaranShanmugam, RamakirushnanSuriyaNarayanan,andVadapalliChandrasekhar MannichBaseLigandsasVersatilePlatformsforSMMs. . . . . . . . . . . . 101 EnriqueColacio Tetrathiafulvalene-BasedMagnetsofLanthanides. . . . . . . . . . . . . . . . . 163 OlivierCadorandFabricePointillart GeometryandMagnetismofLanthanideCompounds. . . . . . . . . . . . . . 191 ZhenhuaZhuandJinkuiTang Single-IonAnisotropy:AnInsighttoComplicated MagneticMolecules. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 227 Shang-DaJiang,Bing-WuWang,andSongGao LanthanideOrganometallicsasSingle-MoleculeMagnets. . . . . . . . . .. . 253 MaríaJoséHerasOjea,LewisC.H.Maddock,andRichardA.Layfield RoleofAbInitioCalculationsintheDesignandDevelopment ofLanthanideBasedSingleMoleculeMagnets. . . . . . . . . . . . . . . . . . . . 281 TulikaGupta,MukeshKumarSingh,andGopalanRajaraman CompleteActiveSpaceWavefunction-BasedAnalysis ofMagnetizationandElectronicStructure. . . . . . . . . . . . . . . . . . . . . . . 355 FrédéricGendron,HélèneBolvin,andJochenAutschbach vii viii Contents MagnetismofActinideCoordinationCompounds. . . . . . . . . . . . . . . . . 391 JanvanLeusen,ManfredSpeldrich,andPaulKögerler Correctionto:Cobalt(II)ComplexesasSingle-IonMagnets. . . . . . . . . . 411 ShaliniTripathi,AtanuDey,MaheswaranShanmugam, RamakirushnanSuriyaNarayanan,andVadapalliChandrasekhar Correctionto:Cobalt(II)/(III)–Lanthanide(III)Complexes asMolecularMagnets. . . . . . .. . . . . . . .. . . . . . .. . . . . . . .. . . . . . . .. 413 AtanuDey,ShaliniTripathi,MaheswaranShanmugam, RamakirushnanSuriyaNarayanan,andVadapalliChandrasekhar Index. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 415 TopOrganometChem(2019)64:1–34 DOI:10.1007/3418_2018_2 #SpringerInternationalPublishingAG2018 Publishedonline:29March2018 – Hybrid Organic Inorganic Cyanide- Bridged Networks TomaszKorzeniak,BeataNowicka,andBarbaraSieklucka Contents 1 Introduction................................................................................... 2 2 MagneticSystems............................................................................. 3 2.1 MagneticInteractions................................................................... 3 2.2 MagneticClusters....................................................................... 4 2.3 MagneticChains........................................................................ 8 2.4 MagneticLayersand3-DNetworks................................................... 10 3 InteractionwithLight......................................................................... 11 3.1 Photomagnetism........................................................................ 11 3.2 Luminescence........................................................................... 17 3.3 Non-linearEffects...................................................................... 19 4 InteractionwithMolecules................................................................... 21 4.1 ReleaseofCoordinatedSolvent........................................................ 21 4.2 GuestMolecules........................................................................ 23 4.3 Guest-ControlledCTandSpin-Crossover............................................. 25 4.4 GuestIons............................................................................... 26 5 Summary...................................................................................... 27 References......................................................................................... 28 Abstract Hybrid organic–inorganic CN-bridged networks are an important and versatile group of molecular magnets. Cyanide ligands mediate relatively strong magneticinteractions and atthe sametimeallow easydesignofpolynuclear assem- blies via building block approach. Introduction of organic ligands allows effective manipulationoftopologyanddimensionality,enablingformationofdiscretepolynu- clear structures, chains and layers as well as intricate 3D architectures. Organic moleculesinhybridsystemscanactasblockingorbridgingligandsaswellasguest molecules. Most importantly, apart from directing the structure formation, organic ligandscanbeusedtoinduceadditionaldesiredproperties.Inthischapter,wepresent numerousexamplesofhybridCN-bridgedassembliestoillustratetheirdiversefunc- tionalities.Theyincludesinglemolecule(SMMs)andsinglechainmagnets(SCMs), T.Korzeniak,B.Nowicka,andB.Sieklucka(*) WydziałChemii,UniwersytetJagielloński,Kraków,Poland e-mail:[email protected]

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