Covalency versus magnetic axiality in Nd molecular magnets: Nd-photoluminescence, strong ligand-field, and unprecedented nephelauxetic effect in fullerenes NdM2N@C80 (M = Sc, Lu, Y)
dc.bibliographicCitation.date | 2024 | |
dc.bibliographicCitation.firstPage | 2141 | |
dc.bibliographicCitation.issue | 6 | |
dc.bibliographicCitation.journalTitle | Chemical Science | eng |
dc.bibliographicCitation.lastPage | 2157 | |
dc.bibliographicCitation.volume | 15 | |
dc.contributor.author | Yang, Wei | |
dc.contributor.author | Rosenkranz, Marco | |
dc.contributor.author | Velkos, Georgios | |
dc.contributor.author | Ziegs, Frank | |
dc.contributor.author | Dubrovin, Vasilii | |
dc.contributor.author | Schiemenz, Sandra | |
dc.contributor.author | Spree, Lukas | |
dc.contributor.author | de Souza Barbosa, Matheus Felipe | |
dc.contributor.author | Guillemard, Charles | |
dc.contributor.author | Valvidares, Manuel | |
dc.contributor.author | Büchner, Bernd | |
dc.contributor.author | Liu, Fupin | |
dc.contributor.author | Avdoshenko, Stanislav M. | |
dc.contributor.author | Popov, Alexey A. | |
dc.date.accessioned | 2024-05-07T11:16:51Z | |
dc.date.available | 2024-05-07T11:16:51Z | |
dc.date.issued | 2023 | |
dc.description.abstract | Nd-based nitride clusterfullerenes NdM2N@C80 with rare-earth metals of different sizes (M = Sc, Y, Lu) were synthesized to elucidate the influence of the cluster composition, shape and internal strain on the structural and magnetic properties. Single crystal X-ray diffraction revealed a very short Nd-N bond length in NdSc2N@C80. For Lu and Y analogs, the further shortening of the Nd-N bond and pyramidalization of the NdM2N cluster are predicted by DFT calculations as a result of the increased cluster size and a strain caused by the limited size of the fullerene cage. The short distance between Nd and nitride ions leads to a very large ligand-field splitting of Nd3+ of 1100-1200 cm−1, while the variation of the NdM2N cluster composition and concomitant internal strain results in the noticeable modulation of the splitting, which could be directly assessed from the well-resolved fine structure in the Nd-based photoluminescence spectra of NdM2N@C80 clusterfullerenes. Photoluminescence measurements also revealed an unprecedentedly strong nephelauxetic effect, pointing to a high degree of covalency. The latter appears detrimental to the magnetic axiality despite the strong ligand field. As a result, the ground magnetic state has considerable transversal components of the pseudospin g-tensor, and the slow magnetic relaxation of NdSc2N@C80 could be observed by AC magnetometry only in the presence of a magnetic field. A combination of the well-resolved magneto-optical states and slow relaxation of magnetization suggests that Nd clusterfullerenes can be useful building blocks for magneto-photonic quantum technologies. | eng |
dc.description.version | publishedVersion | eng |
dc.identifier.uri | https://oa.tib.eu/renate/handle/123456789/14576 | |
dc.identifier.uri | https://doi.org/10.34657/13607 | |
dc.language.iso | eng | |
dc.publisher | Cambridge : RSC | |
dc.relation.doi | https://doi.org/10.1039/d3sc05146c | |
dc.relation.essn | 2041-6539 | |
dc.relation.issn | 2041-6520 | |
dc.rights.license | CC BY 3.0 Unported | |
dc.rights.uri | https://creativecommons.org/licenses/by/3.0 | |
dc.subject.ddc | 540 | |
dc.subject.other | Bond length | eng |
dc.subject.other | Fullerenes | eng |
dc.subject.other | Ligands | eng |
dc.subject.other | Magnetic fields | eng |
dc.subject.other | Neodymium compounds | eng |
dc.subject.other | Photoluminescence | eng |
dc.subject.other | Quantum theory | eng |
dc.subject.other | Rare earths | eng |
dc.subject.other | Single crystals | eng |
dc.subject.other | X ray diffraction | eng |
dc.subject.other | Clusterfullerenes | eng |
dc.subject.other | Covalencies | eng |
dc.subject.other | Different sizes | eng |
dc.subject.other | Internal strains | eng |
dc.subject.other | Ligand-field | eng |
dc.subject.other | Molecular magnet | eng |
dc.subject.other | Nephelauxetic effect | eng |
dc.subject.other | Rare earth metals | eng |
dc.subject.other | Rare-earth metals | eng |
dc.subject.other | Synthesised | eng |
dc.subject.other | Nitrides | eng |
dc.title | Covalency versus magnetic axiality in Nd molecular magnets: Nd-photoluminescence, strong ligand-field, and unprecedented nephelauxetic effect in fullerenes NdM2N@C80 (M = Sc, Lu, Y) | eng |
dc.type | Article | eng |
dc.type | Text | eng |
tib.accessRights | openAccess | |
wgl.contributor | IFWD | |
wgl.subject | Chemie | ger |
wgl.type | Zeitschriftenartikel | ger |
Files
Original bundle
1 - 1 of 1