Manipulating On/Off Single-Molecule Magnet Behavior in a Dy(III)-Based Photochromic Complex

Manipulating On/Off Single-Molecule Magnet Behavior in a Dy(III)-Based Photochromic Complex
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操纵基于 Dy(III) 的光致变色复合物中的开/关单分子磁体行为

DOI:
10.1021/jacs.9b13461
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发表时间:
2020-02-05
影响因子:
15
通讯作者:
Wang, Guo-Ming
Wang, Guo-Ming
中科院分区:
化学1区
文献类型:
--
作者:
Ma, Yu-Juan;Hu, Ji-Xiang;Wang, Guo-Ming

文献摘要

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利用室温(RT)光致变色和光致磁性诱导单分子磁体(SMM)行为在光开关和磁存储器方面具有潜在的应用,并且仍然是开发新的块体磁体的巨大挑战。本文中,一系列链状配合物[Ln(3)(H-HEDP)(3)(H-2-HEDP)(3)]中心点2 H(3)-TPT中心点H-4-HEDP中心点10 H(2)O(QDU-1; Ln = Dy(QDU-1(Dy)),Gd(QDU-1(Gd))和Y(QDU-1(Y)); HEDP =羟基亚乙基二膦酸酯; TPT = 2,4,6-三(4-吡啶基)-1,3,5-三嗪)。所有化合物均表现出可逆的光致变色和光磁行为,通过紫外光照射在室温下,通过光诱导电子转移(PET)机制的光生自由基诱导。更重要的是,PET过程中诱导的Dy(III)同系物的磁相互作用的显着变化。强铁磁耦合与显着缓慢的磁弛豫没有施加直流电场之间的Dy-III离子和光生O-中心点自由基,RT照射后显示SMM行为。首次在镧系材料中观察到了可逆的室温光致变色和光磁性。本工作通过RT光照射实现了自由基驱动的开关SMM行为,为构建光诱导SMM提供了一种新的策略。
Exploitation of room temperature (RT) photochromism and photomagnetism to induce single-molecule magnet (SMM) behavior has potential applications toward optical switches and magnetic memories, and remains a tremendous challenge in the development of new bulk magnets. Herein, a series of chain complexes [Ln(3)(H-HEDP)(3)(H-2-HEDP)(3)]center dot 2H(3)-TPT center dot H-4-HEDP center dot 10H(2)O (QDU-1; Ln = Dy (QDU-1(Dy)), Gd (QDU-1(Gd)), and Y (QDU-1(Y)); HEDP = hydroxyethylidene diphosphonate; TPT = 2,4,6-tri(4-pyridyl)-1,3,5-triazine) were synthesized by solvothermal reactions. All the compounds exhibited reversible photochromic and photomagnetic behaviors via UV light irradiation at RT, induced by the photogenerated radicals via a photoinduced electron transfer (PET) mechanism. More importantly, the PET process induced significant variations in magnetic interactions for the Dy(III) congener. Strong ferromagnetic coupling with remarkably slow magnetic relaxation without applied dc fields was observed between Dy-III ions and photogenerated O-center dot radicals, showing SMM behavior after RT illumination. For the first time, we observed the reversible RT photochromism and photomagnetism in the lanthanide-based materials. This work realized the radicals-actuated on/off SMM behavior via RT light irradiation, providing a new strategy for constructing the light-induced SMMs.