Allouche Florian, Lapadula Giuseppe, Siddiqi Georges, Lukens Wayne W, Maury Olivier, Le Guennic Boris, Pointillart Fabrice, Dreiser Jan, Mougel Victor, Cador Olivier, Copéret Christophe
Department of Chemistry and Applied Biosciences, ETH Zürich , Vladimir Prelog Weg 1-5, CH-8093 Zürich, Switzerland.
Chemical Sciences Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
ACS Cent Sci. 2017 Mar 22;3(3):244-249. doi: 10.1021/acscentsci.7b00035. Epub 2017 Feb 22.
Achieving magnetic remanence at single isolated metal sites dispersed at the surface of a solid matrix has been envisioned as a key step toward information storage and processing in the smallest unit of matter. Here, we show that isolated Dy(III) sites distributed at the surface of silica nanoparticles, prepared with a simple and scalable two-step process, show magnetic remanence and display a hysteresis loop open at liquid He temperature, in contrast to the molecular precursor which does not display any magnetic memory. This singular behavior is achieved through the controlled grafting of a tailored Dy(III) siloxide complex on partially dehydroxylated silica nanoparticles followed by thermal annealing. This approach allows control of the density and the structure of isolated, "bare" Dy(III) sites bound to the silica surface. During the process, all organic fragments are removed, leaving the surface as the sole ligand, promoting magnetic remanence.
在固体基质表面分散的单个孤立金属位点上实现磁剩磁,被视为朝着以物质的最小单位进行信息存储和处理迈出的关键一步。在此,我们表明,通过简单且可扩展的两步法制备的二氧化硅纳米颗粒表面分布的孤立Dy(III)位点,呈现出磁剩磁,并在液氦温度下显示出一个开放的磁滞回线,这与不显示任何磁记忆的分子前驱体形成对比。这种独特的行为是通过将定制的Dy(III)硅氧化物配合物可控接枝到部分脱羟基的二氧化硅纳米颗粒上,然后进行热退火来实现的。这种方法能够控制与二氧化硅表面结合的孤立“裸露”Dy(III)位点的密度和结构。在此过程中,所有有机片段都被去除,仅留下表面作为唯一配体,从而促进了磁剩磁。