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31.
Dr. Yoji Horii Dr. Keiichi Katoh Dr. Kunihisa Sugimoto Dr. Ryo Nakanishi Dr. Brian K. Breedlove Prof. Dr. Masahiro Yamashita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(12):3098-3104
In the research field of single-molecule magnets (SMMs), lanthanoid–lanthanoid interactions, so-called f–f interactions, are known to affect the SMM properties, although their magnitudes are small. In this article, an SMM with very weak f–f interactions is reported, and the effects of the interactions on the SMM properties are discussed. X-ray structural analysis of the DyIII-CdII-phthalocyaninato sextuple-decker complex (Dy2Cd3) reveals that the intramolecular Dy−Dy length in Dy2Cd3 is more than 13 Å, which is longer than the intermolecular Dy−Dy length. Even though the two DyIII ions are far apart, intermolecular ferromagnetic dipole–dipole interactions are observed in Dy2Cd3. From detailed analysis of ac magnetic susceptibilities, quantum tunneling of the magnetization (QTM) in Dy2Cd3 is partially suppressed owing to the existence of very weak Dy−Dy interactions. Our results show that even very weak Dy−Dy interactions act as a dipolar bias, suppressing QTM. 相似文献
32.
Eva Lucaccini Matteo Briganti Dr. Mauro Perfetti Dr. Laure Vendier Dr. Jean‐Pierre Costes Dr. Federico Totti Prof. Dr. Roberta Sessoli Prof. Dr. Lorenzo Sorace 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(16):5552-5562
The magnetic behaviour of a Dy(LH)3 complex (LH? is the anion of 2‐hydroxy‐N′‐[(E)‐(2‐hydroxy‐3‐methoxyphenyl)methylidene]benzhydrazide) was analysed in depth from both theoretical and experimental points of view. Cantilever torque magnetometry indicated that the complex has Ising‐type anisotropy, and provided two possible directions for the easy axis of anisotropy due to the presence of two magnetically non‐equivalent molecules in the crystal. Ab initio calculations confirmed the strong Ising‐type anisotropy and disentangled the two possible orientations. The computed results obtained by using ab initio calculations were then used to rationalise the composite dynamic behaviour observed for both pure DyIII phase and YIII diluted phase, which showed two different relaxation channels in zero and non‐zero static magnetic fields. In particular, we showed that the relaxation behaviour at the higher temperature range can be correctly reproduced by using a master matrix approach, which suggests that Orbach relaxation is occurring through a second excited doublet. 相似文献
33.
Ikjin Kim Dr. Avinash Dhamija Dr. In-Chul Hwang Hochan Lee Dr. Young Ho Ko Prof. Dr. Kimoon Kim 《化学:亚洲杂志》2021,16(20):3209-3212
Here, we report the synthesis of a truncated cone-shaped triangular porphyrinic macrocycle, P3L3 , via a single step imine condensation of a cis-diaminophenylporphyrin and a bent dialdehyde-based linker as building units. X-ray diffraction analysis reveals that the truncated cone-shaped P3L3 molecules are stacked on top of each other by π⋯π and CH⋯π interactions, to form 1.7 nm wide hollow columns in the solid state. The formation of the triangular macrocycle is corroborated by quantum chemical calculations. The permanent porosity of the P3L3 crystals is demonstrated by several gas sorption experiments and powder X-ray diffraction analysis. 相似文献
34.
Sergei V. Chapyshev Denis V. Korchagin Paulo Costa Wolfram Sander 《Magnetic resonance in chemistry : MRC》2022,60(8):829-835
The first X-band EPR spectrum containing only non-overlapping signals of septet pyridyl-2,4,6-trinitrene and triplet pyridylnitrenes is reported. This spectrum was recorded after photolysis of 2,4,6-triazidopyridine in solid argon at 5 K. The zero-field splitting (ZFS) parameters of this trinitrene as well as of intermediate triplet mononitrenes and quintet dinitrenes formed at early stages of the photolysis were determined using the combination of modern computer line-shape spectral simulations and density functional theory (DFT) calculations. It was found that septet pyridyl-2,4,6-trinitrene has the record negative parameter DS = −0.1031 cm−1 among all known to date septet pyridyl-2,4,6-trinitrenes and may be of interest as a model multi-qubit spin system for investigations of quantum computation processing. 相似文献
35.
Enantioselective Self‐Assembly of Triangular Dy3 Clusters with Single‐Molecule Magnet Behavior 下载免费PDF全文
Three pairs of enantiopure chiral triangular Ln3 clusters, [Ln3LRRRRRR/SSSSSS(μ3‐OH)2(H2O)2(SCN)4]?xCH3OH?yH2O ( R ‐Dy3 , Ln=Dy, x=6, y=0; S ‐Dy3 , Ln=Dy, x=6, y=1; R ‐Ho3 , Ln=Ho, x=6, y=1; S ‐Ho3 , Ln=Ho, x=6, y=1; R ‐Er3 , Ln=Er, x=6, y=0; S ‐Er3 , Ln=Er, x=6, y=1), have been successfully synthesized by a rational enantioselective synthetic strategy. The core of triangular Ln3 is bound in the central N6O3 of the macrocyclic ligand, and the coordination spheres of Ln ions are completed by four SCN? anions and two H2O molecules in axial positions of the macrocycle. The circular dichroism (CD) and vibrational circular dichroism (VCD) spectra of the enantiomers demonstrate that the chirality is successfully transferred from the ligands to the resulting Ln3 clusters. Ac susceptibility measurements reveal that single‐molecule magnet behavior occurs for both enantiopure clusters of R ‐Dy3 and S ‐Dy3 . This work is one of the few examples of the successful design of a pair of triangular Dy3 clusters showing simultaneously slow magnetic relaxation and optical activity, and this might open up new opportunities to develop novel multifunctional materials. 相似文献
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40.
Haiquan Tian Dr. Lang Zhao Haifeng Lin Prof. Dr. Jinkui Tang Prof. Dr. Guangshe Li 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(39):13235-13241
Two new “butterfly‐shaped” pentanuclear dysprosium(III) clusters, [Dy5(μ3‐OH)3(opch)6(H2O)3] ? 3 MeOH ? 9 H2O ( 1 ) and [Dy5(μ3‐OH)3(Hopch)2(opch)4(MeOH)(H2O)2] ? (ClO4)2 ? 6 MeOH ? 4 H2O ( 2 ), which were based on the heterodonor‐chelating ligand o‐vanillin pyrazine acylhydrazone (H2opch), have been successfully synthesized by applying different reaction conditions. Single‐crystal X‐ray diffraction analysis revealed that the butterfly‐shaped cores in both compounds were comparable. However, their magnetic properties were drastically different. Indeed, compound 1 showed dual slow‐relaxation processes with a transition between them that corresponded to energy gaps (Δ) of 8.1 and 37.9 K and pre‐exponential factors (τ0) of 1.7×10?5 and 9.7×10?8 s for the low‐ and high‐temperature domains, respectively, whilst only a single relaxation process was noted for compound 2 (Δ=197 K, τ0=3.2×10?9 s). These significant disparities are most likely due to the versatile coordination of the H2opch ligands with particular keto–enol tautomerism, which alters the strength of the local crystal field and, hence, the nature or direction of the easy axes of anisotropic dysprosium ions. 相似文献