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Homochiral Dy2 single-molecule magnets with strong magneto-optical Faraday effects and strong third-harmonic generation
Inorganic Chemistry Frontiers ( IF 7 ) Pub Date : 2024-04-17 , DOI: 10.1039/d4qi00691g Cai-Ming Liu 1 , Rong Sun 2 , Xiang Hao 1 , Xi-Li Li 3 , Bing-Wu Wang 2
Inorganic Chemistry Frontiers ( IF 7 ) Pub Date : 2024-04-17 , DOI: 10.1039/d4qi00691g Cai-Ming Liu 1 , Rong Sun 2 , Xiang Hao 1 , Xi-Li Li 3 , Bing-Wu Wang 2
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Four pairs of homochiral Dy2 complexes were directionally prepared using homochiral β-diketone ligands {D-Htfc/L-Htfc = (+)/(−)-3-trifluoroacetyl camphor, D-Hpfc/L-Hpfc = 3-(perfluorobutyryl)-(+)/(−)-camphor} and hydrazone Schiff base bridging ligands {H2L1 = (E)-N’-(2-hydroxy-3-methoxybenzylidene)pyrazine-2-carbohydrazide, H2L2 = (E)-N’-(2-hydroxy-3-methoxybenzylidene)nicotinohydrazide} at room temperature: [Dy2(D-tfc/L-tfc)2(L1)2(H2O)2]·2DMF (D-1/L-1), [Dy2(D-tfc/L-tfc)2(L2)2(H2O)2]·2DMF (D-2/L-2), [Dy2(D-pfc/L-pfc)2(L1)2(DMF)2] (D-3/L-3), and [Dy2(D-pfc/L-pfc)2(L2)2(H2O)2]·2DMF (D-4/L-4). These enantiomers show intramolecular ferromagnetic interactions between Dy3+ ions and exhibit good single-molecule magnet (SMM) properties at a zero dc field, with Ueff/k values of 47.6 K, 152.2 K, 173.8 K and 116.2 K for D-1, D-2, D-3 and D-4, respectively. These magnetic properties were explained with ab initio calculations. The magnetic circular dichroism (MCD) investigation revealed that these four pairs of enantiomers have strong magneto-optical Faraday effects. Besides the second harmonic generation (SHG), they exhibit surprisingly strong third harmonic generation (THG). Notably, the magnetic properties, magneto-optical properties and nonlinear optical properties of such homochiral SMMs can be adjusted by the functional groups on the ligands. Among them, D-1/L-1 has the potential for applications in magneto-optical and/or nonlinear optical materials or devices due to its strongest THG intensity (661.8 × α-SiO2) and strongest magneto-optical Faraday effect.
中文翻译：
具有强磁光法拉第效应和强三次谐波产生的同手性 Dy2 单分子磁体
使用纯手性β-二酮配体定向制备四对纯手性Dy 2配合物{ D -Htfc/ L -Htfc = (+)/(−)-3-三氟乙酰樟脑，D -Hpfc/ L -Hpfc = 3-(全氟丁酰基) )-(+)/(−)-樟脑}和腙席夫碱桥联配体{H 2 L1 = ( E )- N' -(2-羟基-3-甲氧基亚苄基)吡嗪-2-碳酰肼， H 2 L2 = ( E )- N' -(2-羟基-3-甲氧基亚苄基)烟酰肼}在室温下：[Dy 2 ( D -tfc/ L -tfc) 2 (L1) 2 (H 2 O) 2 ]·2DMF ( D - 1 / L -1 ), [Dy 2 ( D -tfc/ L -tfc) 2 (L2) 2 (H 2 O) 2 ]·2DMF ( D -2 / L -2 ), [Dy 2 ( D -pfc) / L -pfc) 2 (L1) 2 (DMF) 2 ] ( D -3 / L -3 ) 和 [Dy 2 ( D -pfc/ L -pfc) 2 (L2) 2 (H 2 O) 2 ] ·2DMF（D -4 / L -4）。这些对映体表现出 Dy 3+离子之间的分子内铁磁相互作用，并在零直流场下表现出良好的单分子磁体 (SMM) 特性，D -1的U eff / k值为 47.6 K、152.2 K、173.8 K 和 116.2 K 、D -2、D -3和D -4。这些磁性特性是通过从头计算来解释的。磁圆二色性（MCD）研究表明，这四对对映体具有很强的磁光法拉第效应。除了二次谐波产生 (SHG) 之外，它们还表现出令人惊讶的强大三次谐波产生 (THG)。值得注意的是，这种纯手性SMM的磁特性、磁光特性和非线性光学特性可以通过配体上的官能团进行调节。其中，D -1 /L -1由于其最强的THG强度（661.8×α-SiO 2）和最强的磁光法拉第效应，在磁光和/或非线性光学材料或器件中具有应用潜力
更新日期：2024-04-17
中文翻译：
具有强磁光法拉第效应和强三次谐波产生的同手性 Dy2 单分子磁体
使用纯手性β-二酮配体定向制备四对纯手性Dy 2配合物{ D -Htfc/ L -Htfc = (+)/(−)-3-三氟乙酰樟脑，D -Hpfc/ L -Hpfc = 3-(全氟丁酰基) )-(+)/(−)-樟脑}和腙席夫碱桥联配体{H 2 L1 = ( E )- N' -(2-羟基-3-甲氧基亚苄基)吡嗪-2-碳酰肼， H 2 L2 = ( E )- N' -(2-羟基-3-甲氧基亚苄基)烟酰肼}在室温下：[Dy 2 ( D -tfc/ L -tfc) 2 (L1) 2 (H 2 O) 2 ]·2DMF ( D - 1 / L -1 ), [Dy 2 ( D -tfc/ L -tfc) 2 (L2) 2 (H 2 O) 2 ]·2DMF ( D -2 / L -2 ), [Dy 2 ( D -pfc) / L -pfc) 2 (L1) 2 (DMF) 2 ] ( D -3 / L -3 ) 和 [Dy 2 ( D -pfc/ L -pfc) 2 (L2) 2 (H 2 O) 2 ] ·2DMF（D -4 / L -4）。这些对映体表现出 Dy 3+离子之间的分子内铁磁相互作用，并在零直流场下表现出良好的单分子磁体 (SMM) 特性，D -1的U eff / k值为 47.6 K、152.2 K、173.8 K 和 116.2 K 、D -2、D -3和D -4。这些磁性特性是通过从头计算来解释的。磁圆二色性（MCD）研究表明，这四对对映体具有很强的磁光法拉第效应。除了二次谐波产生 (SHG) 之外，它们还表现出令人惊讶的强大三次谐波产生 (THG)。值得注意的是，这种纯手性SMM的磁特性、磁光特性和非线性光学特性可以通过配体上的官能团进行调节。其中，D -1 /L -1由于其最强的THG强度（661.8×α-SiO 2）和最强的磁光法拉第效应，在磁光和/或非线性光学材料或器件中具有应用潜力
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