Abstract:Single-ion magnets (SIMs) and single-molecule magnets (SMMs) are typically made up of 3d and/or 4f complexes that possess significant energy barriers to prevent the spin reversal behavior at the molecular...
“…Single-molecule magnets (SMMs) have attracted considerable attention in the field of information storage and luminescent thermometers because they can retain unquenched orbital angular momentum and are molecular materials. − Generally, Ln III ions have larger unquenchable orbital angular momentum and greater anisotropy compared to transition metals. Therefore, they are favorable candidates for constructing high-performance SMMs. − Usually, the parameters used to evaluate the performance of SMMs are a highly effective energy barrier ( U eff ) and blocking temperature ( T B ). − In the last 20 years, researchers have synthesized many complexes with different nuclear numbers: mononuclear, binuclear, tetranuclear, and hexanuclear. Of these, most studies have focused on mononuclear SMMs due to their simplicity as models for probing magneto-structural correlations. , In the most notable result, Layfield et al synthesized a mononuclear complex which T B broke the limit of liquid nitrogen .…”
Using the Schiff base ligand H 2 L-pyra (N′-(2hydroxybenzoyl)pyrazine-2-carbohydrazonamide) with multiple dentate sites, the trinuclear Dy III -based complex [Dy 3 (HLpyra) 2 (L-pyra) 2 (CH 3 COO) 3 ]•2H 2 O (1) was synthesized. By analyzing the fragmented assembly process and fine-tuning the b r i d g i n g a n i o n s , c o m p l e x [ D y 4 ( H L -p y r a ) 2 ( L -p y ra) 4 2) with different nuclear numbers was successfully synthesized. Magnetic studies demonstrated that 1 did not exhibit magnetic relaxation behavior under the external field; however, 2 exhibited zero-field single-molecule magnetic relaxation behavior with an effective energy barrier (U eff ) of 197.44 K. This is attributed to the improved anisotropy of the single ion after the normalization of the crystal structure, thus realizing the molecular magnetic switching. Moreover, magnetic dilution analysis of 2 demonstrated that the weak magnetic interaction between metal ions inhibited the occurrence of quantum tunneling of magnetization (QTM), resulting in high-performance single-molecule magnet (SMM) behavior. The reasons for the magnetic difference between these two complexes were analyzed using ab initio calculation and magneto-structural correlations. This study provides a reasonable prediction of the ideal configuration of the approximately parallelogram Dy III -based SMMs, thus offering an effective approach for synthesizing Dy 4 complexes with excellent properties.
“…[1][2][3][4][5][6][7][8] Since the first Ln-SMM {TbPc 2 } was discovered in 2003, 9 a great number of lanthanide-based SMMs have been prepared and investigated in subsequent surveys, owing to the high-spin ground state and unquenched orbital angular momentum of lanthanide ions. [10][11][12][13][14] To obtain SMMs with good performance, a great number of efforts have been made to create lanthanide systems: for example, the dysprosium metallocene [(Cp ttt ) 2 Dy][B (C 6 F 5 ) 4 ] (Cp ttt = 1,2,4-tri-tert-butylcyclopentadienyl) 15 and [(Cp iPr5 ) Dy(Cp*)] + (Cp iPr5 = pentaisopropylcyclopentadienyl; Cp* = pentamethylcyclopentadienyl). 16 However, obvious quantum tunneling of magnetization (QTM) usually exists in the lanthanide-based SMMs, which is a disadvantage for obtaining high energy barriers.…”
Two LnIII complexes Ln(HTMSA)3(H2O)25.5H2O (Ln = Dy (1) and Tb (2), H2TMSA = 5-azotriazolyl-3-methoxysalicylaldehyde) and two MnII-LnIII cluster [Mn(H2O)6][MnLn2(TTMSA)4(HTTMSA)2(H2O)6]4H2O (Ln = Dy (3) and Tb (4), H2TTMSA = 5-azotetrazolyl-3-methoxysalicylaldehyde) have...
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