通过选择性吸收铁来恢复Co卟啉阵列的界面Co磁矩
Restoring the Co Magnetic Moments at Interfacial Co-Porphyrin Arrays by Site-Selective Uptake of Iron
作者:Saranyan Vijayaraghavan;Willi Auwärter;David Ecija;Knud Seufert;Stefano Rusponi;Torsten Houwaart;Philippe Sautet;Marie-Laure Bocquet;Pardeep Thakur;Sebastian Stepanow;Uta Schlickum;Markus Etzkorn;Hara
关键词:magnetochemistry,magnetic moment,metalloporphyrin,template,scanning tunneling microscopy (STM),X-ray magneticShow More
DOI:https://doi.org/10.1021/nn507346x
发表时间:2015年
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摘要
磁化学最近出现为控制表面上可寻址自旋阵列的有前途的方法。在这里,我们报告了铁在高度规则的四苯基卟啉钴(Co-TPP)模板上的结合、空间排序和磁性质,并强调了铁如何控制钴中心的磁性。通过扫描隧道显微镜(STM)观察到,单个铁原子选择性地附着在一个由Co-N-C-C-C-N循环亚单位定义的七聚体中的鞍状构象位置上,提供了一个独特的配位环境。尽管裸露的Co-TPP/Ag(111)的钴的磁矩被熄灭,但铁的存在重新激活了它。我们的X射线磁圆二色性(XMCD)实验证明,铁和钴中心之间存在铁磁偶合,伴随着涉及卟啉配体的复杂电荷重分布,这得到了密度泛函理论(DFT)计算的支持。因此,我们展示了一种不寻常的金属卟啉配位几何,为在基于表面的纳米结构中空间排序和工程磁矩开辟了途径。
Abstract
Magnetochemistry recently emerged as a promising approach to control addressable spin arrays on surfaces. Here we report on the binding, spatial ordering, and magnetic properties of Fe on a highly regular Co-tetraphenylporphyrin (Co-TPP) template and highlight how the Fe controls the magnetism of the Co centers. As evidenced by scanning tunneling microscopy (STM) single Fe atoms attach to the saddle-shape conformers site-selectively in a unique coordination environment offered through a heptamer defined by the Co–N–C–C–C–N cyclic subunit. While the magnetic moment of Co is quenched for bare Co-TPP/Ag(111), the Fe presence revives it. Our X-ray magnetic circular dichroism (XMCD) experiments, complemented by density functional theory (DFT) calculations, evidence a ferromagnetic coupling between the Fe and the Co center concomitant with a complex charge redistribution involving the porphyrin ligand. Thus, we demonstrate an unusual metalloporphyrin coordination geometry that opens pathways to spatially order and engineer magnetic moments in surface-based nanostructures.
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