Pineda Eufemio Moreno, Lan Yanhua, Fuhr Olaf, Wernsdorfer Wolfgang, Ruben Mario
Institute of Nanotechnology (INT) , Karlsruhe Institute of Technology (KIT) , Hermann-von-Helmholtz-Platz 1, D-76344 Eggenstein-Leopoldshafen , Germany . Email:
Institut Néel , CNRS , Université Grenoble Alpes , 25 rue des Martyrs , F-38000 Grenoble , France.
Chem Sci. 2017 Feb 1;8(2):1178-1185. doi: 10.1039/c6sc03184f. Epub 2016 Sep 22.
Carbamate formation in green-plants through the RuBisCO enzyme continuously plays a pivotal role in the conversion of CO from the atmosphere into biomass. With this in mind, carbamate formation from CO by a lanthanide source in the presence of a secondary amine is herein explored leading to a lanthanide-carbamate cage with the formula [Dy(OCNPr)]. Magnetic studies show slow relaxation leading to the observation of hysteresis loops; the tetranuclear cage being a single molecule magnet. Detailed interpretation of the data reveals: (i) the presence of two different exchange interactions, ferromagnetic and antiferromagnetic and (ii) the observation of exchange-bias quantum tunnelling with two distinct sets of loops, attributable to ferromagnetic interactions between dysprosium ions at longer distances and antiferromagnetic exchange between dysprosium ions at shorter distances. The results clearly demonstrate that the [Dy(OCNPr)] cage acts as a quantum magnet which in turn could be at the heart of hybrid spintronic devices after having implemented CO as a feedstock.
通过核酮糖-1,5-二磷酸羧化酶(RuBisCO)在绿色植物中形成氨基甲酸盐,在将大气中的二氧化碳转化为生物质的过程中持续发挥着关键作用。考虑到这一点,本文探索了在仲胺存在下由镧系元素源从二氧化碳形成氨基甲酸盐,从而得到分子式为[Dy(OCNPr)]的镧系氨基甲酸盐笼。磁性研究表明弛豫缓慢,从而观察到磁滞回线;该四核笼是一种单分子磁体。对数据的详细解释揭示:(i)存在两种不同的交换相互作用,铁磁和反铁磁,以及(ii)观察到具有两组不同回线的交换偏置量子隧穿,这归因于较长距离处镝离子之间的铁磁相互作用和较短距离处镝离子之间的反铁磁交换。结果清楚地表明,[Dy(OCNPr)]笼作为一种量子磁体,在将二氧化碳用作原料后,反过来可能成为混合自旋电子器件的核心。