Single-molecule magnets(SMMs)are promising candidates as components for the next generation of molecule-based electronics.As the state-of-the-art in this field is mainly focused on heavy lanthanide(III)(Ln^(III))ions,...Single-molecule magnets(SMMs)are promising candidates as components for the next generation of molecule-based electronics.As the state-of-the-art in this field is mainly focused on heavy lanthanide(III)(Ln^(III))ions,examples of light lanthanide-based systems,e.g.,those based on Nd^(III),have fallen far behind.Besides the slow relaxation of magnetisation,the luminescence of multifunctional Ln^(III) complexes can be leveraged for in situ temperature monitoring via luminescence thermometry.To help understand how both magnetic and luminescence performance can be improved through structural modifications in Nd^(III)-based SMMs,two dinuclear Nd^(III) complexes,[Nd^(III)_(2)(valdien)_(2)(X)_(2)](X=acac-{1-Nd_(2)}or NO_(3)-{2-Nd_(2)}),are herein reported,and we discuss opto-and magneto-structural correlations depending on the terminal ligand.The Nd^(III) complexes display field-induced slow relaxation of magnetization,but for{2-Nd_(2)},QTM has a lower contribution because the longer Nd^(III)-Oterminal distances induce a weaker equatorial crystal field component.The systems were further used to develop luminescent temperature probes featuring a maximum thermal sensitivity of 0.52%K-1 at 40 K for{2-Nd_(2)},confirming its multifunctional slow relaxation of magnetisation and temperature readout features.展开更多
基金financial support provided by the University of Ottawa,the Canadian Foundation for Innovation(CFI),and the Natural Sciences and Engineering Research Council of Canada(NSERC)A.G.B.J.acknowledges the São Paulo Research Foundation FAPESP(Grant No.2021/09755-0 and 2019/23763-6)+2 种基金F.A.S.acknowledges FAPESP:2021/06326-1 and 2021/08111-2,INCT/INOMAT-National Institute of Science Technology in Complex Functional Materials(CNPq:465452/2014-0 and FAPESP:50906-9/2014)FAPESP:2012/11382-9,and CNPq 306107/2019-8Claudia Calado Dias is acknowledged for powder XRD measurements and Alexandros A.Kitos for useful discussions.
文摘Single-molecule magnets(SMMs)are promising candidates as components for the next generation of molecule-based electronics.As the state-of-the-art in this field is mainly focused on heavy lanthanide(III)(Ln^(III))ions,examples of light lanthanide-based systems,e.g.,those based on Nd^(III),have fallen far behind.Besides the slow relaxation of magnetisation,the luminescence of multifunctional Ln^(III) complexes can be leveraged for in situ temperature monitoring via luminescence thermometry.To help understand how both magnetic and luminescence performance can be improved through structural modifications in Nd^(III)-based SMMs,two dinuclear Nd^(III) complexes,[Nd^(III)_(2)(valdien)_(2)(X)_(2)](X=acac-{1-Nd_(2)}or NO_(3)-{2-Nd_(2)}),are herein reported,and we discuss opto-and magneto-structural correlations depending on the terminal ligand.The Nd^(III) complexes display field-induced slow relaxation of magnetization,but for{2-Nd_(2)},QTM has a lower contribution because the longer Nd^(III)-Oterminal distances induce a weaker equatorial crystal field component.The systems were further used to develop luminescent temperature probes featuring a maximum thermal sensitivity of 0.52%K-1 at 40 K for{2-Nd_(2)},confirming its multifunctional slow relaxation of magnetisation and temperature readout features.
