Chen Chia-Hsiang, Spree Lukas, Koutsouflakis Emmanouil, Krylov Denis S, Liu Fupin, Brandenburg Ariane, Velkos Georgios, Schimmel Sebastian, Avdoshenko Stanislav M, Fedorov Alexander, Weschke Eugen, Choueikani Fadi, Ohresser Philippe, Dreiser Jan, Büchner Bernd, Popov Alexey A
Leibniz Institute for Solid State and Materials Research Helmholtzstraße 20 Dresden 01069 Germany.
Department of Medicinal and Applied Chemistry Kaohsiung Medical University Kaohsiung 807 Taiwan.
Adv Sci (Weinh). 2021 Jan 21;8(5):2000777. doi: 10.1002/advs.202000777. eCollection 2021 Mar.
Tremendous progress in the development of single molecule magnets (SMMs) raises the question of their device integration. On this route, understanding the properties of low-dimensional assemblies of SMMs, in particular in contact with electrodes, is a necessary but difficult step. Here, it is shown that fullerene SMM self-assembled on metal substrate from solution retains magnetic hysteresis up to 10 K. Fullerene-SMM DyScN@C and DyScN@C are derivatized to introduce a thioacetate group, which is used to graft SMMs on gold. Magnetic properties of grafted SMMs are studied by X-ray magnetic circular dichroism and compared to the films of nonderivatized fullerenes prepared by sublimation. In self-assembled films, the magnetic moments of the Dy ions are preferentially aligned parallel to the surface, which is different from the disordered orientation of endohedral clusters in nonfunctionalized fullerenes. Whereas chemical derivatization reduces the blocking temperature of magnetization and narrows the hysteresis of DyScN@C, for DyScN@C equally broad hysteresis is observed as in the fullerene multilayer. Magnetic bistability in the DyScN@C grafted on gold is sustained up to 10 K. This study demonstrates that self-assembly of fullerene-SMM derivatives offers a facile solution-based procedure for the preparation of functional magnetic sub-monolayers with excellent SMM performance.
单分子磁体(SMMs)发展取得的巨大进展引发了其器件集成的问题。在这条道路上,了解SMMs低维组装体的性质,特别是与电极接触时的性质,是必要但困难的一步。在此,研究表明从溶液中自组装在金属基底上的富勒烯SMM在高达10 K时仍保留磁滞现象。富勒烯-SMM DyScN@C和DyScN@C经衍生化引入硫代乙酸酯基团,用于将SMMs接枝到金上。通过X射线磁圆二色性研究接枝SMMs的磁性,并与通过升华制备的未衍生化富勒烯薄膜进行比较。在自组装薄膜中,Dy离子的磁矩优先平行于表面排列,这与未功能化富勒烯中内包簇的无序取向不同。虽然化学衍生化降低了磁化的阻塞温度并缩小了DyScN@C的磁滞,但对于DyScN@C,观察到与富勒烯多层膜中同样宽的磁滞。接枝在金上的DyScN@C中的磁双稳性在高达10 K时得以维持。这项研究表明,富勒烯-SMM衍生物的自组装为制备具有优异SMM性能的功能性磁性亚单层提供了一种简便的基于溶液的方法。