Formation of a G-quartet-Fe complex and modulation of electronic and magnetic properties of the Fe center.
Formation of a G-quartet-Fe complex and modulation of electronic and magnetic properties of the Fe center.
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DOI：
10.1021/nn5054156
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发表时间：
2014-10
期刊：
影响因子：
17.1
通讯作者：
Likun Wang;Huihui Kong;Chi Zhang;Qiang Sun;L. Cai;Qinggang Tan;F. Besenbacher;W. Xu
中科院分区：
文献类型：
--
作者：
Likun Wang;Huihui Kong;Chi Zhang;Qiang Sun;L. Cai;Qinggang Tan;F. Besenbacher;W. Xu
尽管G-四重体结构因其重要的生物学意义而被广泛研究，但孤立的G-四重体在固体表面的形成机制，特别是金属中心的必要性仍然不明确。在这里，通过使用控制良好的超高真空条件下的扫描隧道显微镜和密度泛函理论计算，我们已经能够澄清，除了四重态之间的氢键之外，金属中心对于孤立的G-四重态的形成是必不可少的。此外，通过局部纳米尺度的扫描隧道显微镜操作，通过微妙地扰动形成的G-四重态络合物中的局域配位键合方案，我们成功地调制了d轨道和伴随的金属中心的磁性。我们的结果证明了在固体表面形成孤立的G-四重态络合物的可行性，并且这种调节金属中心的电学和磁学性质的策略可以推广到其他相关的系统，如分子自旋电子学。
Although the G-quartet structure has been extensively investigated due to its biological importance, the formation mechanism, in particular, the necessity of metal centers, of an isolated G-quartet on solid surfaces remains ambiguous. Here, by using scanning tunneling microscopy under well-controlled ultra-high-vacuum conditions and density functional theory calculations we have been able to clarify that besides the intraquartet hydrogen bonding a metal center is mandatory for the formation of an isolated G-quartet. Furthermore, by subtly perturbing the local coordination bonding schemes within the formed G-quartet complex via local nanoscale scanning tunneling microscopy manipulations, we succeed in modulating the d orbitals and the accompanying magnetic properties of the metal center. Our results demonstrate the feasibility of forming an isolated G-quartet complex on a solid surface and that the strategy of modulating electronic and magnetic properties of the metal center can be extended to other related systems such as molecular spintronics.