Combined experimental and theoretical studies on a series of mononuclear LnIII single-molecule magnets: dramatic influence of remote substitution on the magnetic dynamics in Dy analogues
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15310%2F23%3A73621961" target="_blank" >RIV/61989592:15310/23:73621961 - isvavai.cz</a>
Result on the web
<a href="https://pubs.rsc.org/en/content/articlelanding/2023/dt/d2dt03354b" target="_blank" >https://pubs.rsc.org/en/content/articlelanding/2023/dt/d2dt03354b</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1039/d2dt03354b" target="_blank" >10.1039/d2dt03354b</a>
Alternative languages
Result language
angličtina
Original language name
Combined experimental and theoretical studies on a series of mononuclear LnIII single-molecule magnets: dramatic influence of remote substitution on the magnetic dynamics in Dy analogues
Original language description
A series of Ln(III) complexes of general formula [Ln(H2L1)(2)(NO3)(2)(H2O)](NO3) (1-5) [Ln = Dy (1), Tb (2) Ho (3), Er (4), and Yb (5)] and an analogous Dy-III complex with ligand H2L2, [Dy(H2L2)(2)(NO3)(3)(H2O)](NO3) (6), where H2L1 and H2L2 stand for (E)-2-[(2-hydroxyphenyl)iminomethyl]-6-methoxy-4-methylphenol and (E)-2-[(2-hydroxy-5-methylphenyl)iminomethyl]-6-methoxy-4-methylphenol, respectively, have been synthesized and magneto-structurally characterized. All these complexes are isostructural and isomorphous, in which the zwitterionic form of the ligands predominantly coordinate the metal centers. The magnetic study revealed that complex 3 displays negligible SMM behaviour, while 1 and 6 are zero field SMMs, the performance of which can largely be improved in the presence of an applied dc field by lowering under barrier relaxation processes, and finally 2, 4, and 5 are field-induced SMMs. The most remarkable observation in the present study is the dramatically-enhanced SMM performance in 6 compared to 1, achieved by only a remote methyl substitution at the ligand framework to increase the intermolecular separation. Although SINGLE_ANISO ab initio calculations for 1 and 6 are very similar, the POLY_ANISO module revealed weak dipolar interactions in both the compounds but significant antiferromagnetic interaction in 1, thereby justifying the experimental fact. The present work discloses that even a small substitution such as a methyl group can adequately increase the intermolecular separation, leading to several-fold enhanced effective energy barrier.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10402 - Inorganic and nuclear chemistry
Result continuities
Project
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Continuities
I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Others
Publication year
2023
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Dalton Transactions
ISSN
1477-9226
e-ISSN
1477-9234
Volume of the periodical
52
Issue of the periodical within the volume
5
Country of publishing house
GB - UNITED KINGDOM
Number of pages
16
Pages from-to
1241-1256
UT code for WoS article
000909508800001
EID of the result in the Scopus database
2-s2.0-85146152889