锕系原子修饰的gh-C3N4单层优良5f电子磁体,Physical Chemistry Chemical Physics

当前位置： X-MOL 学术 › Phys. Chem. Chem. Phys. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

锕系原子修饰的gh-C3N4单层优良5f电子磁体
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2023-09-30 , DOI: 10.1039/d3cp02954a
Tao Xiong ₁ , Yaqing Chen ₁ , Ruizhi Qiu ₂ , Hongkuan Yuan _{1,

3}

Affiliation

二维（2D）材料的原子功能，通常具有可控的掺杂途径，可提供规则的原子排列以及优异的磁性，对于基础研究和自旋电子学应用都至关重要。在这里，探索了5f 电子锕系元素 (An = Ac-Am) 在多孔石墨烯类碳氮化物 (gh-C ₃ N ₄ ) 层上的吸附，以确定其结构稳定性、电子性质和磁性。密度泛函理论 (DFT) 计算、从头算分子动力学 (AIMD)、蒙特卡罗 (MC) 模拟和化学键分析的结合。_{我们的研究表明，每个 An 原子可以单独吸附在 gh-C 3} N ₄片的空位位点上，具有高能量、热和动力学稳定性，这源于离子 An-N 键合的主要相互作用以及次要相互作用。 An-5f6d 态与 N-2s2p 态共价键的相互作用。极少数 5f 电子的离域取决于它们是否占据与形成 5f-2s2p 共价键的配体轨道匹配并有助于杂交的亚轨道。我们提出，Ruderman-Kittel-Kasuya-Yosida (RKKY) 机制对于通过6d 电子作为传导电子的原子间 5f-5f 磁交换起着决定性作用。来自局域 5f 电子的大磁矩和磁各向异性能量 (MAE)，加上离域 6d 电子带来的金属特性，使这些 An 基 2D 材料成为优异的金属磁体，特别是对于 U@gh-C ₃ N ₄该系统具有 0.6 μB的适度磁矩、53 meV 的大 MAE 和₅₃₈ K 的高居里温度 ( T _C )。

"点击查看英文标题和摘要"

Excellent 5f-electron magnet of actinide atom decorated gh-C3N4 monolayer

Atomic functionality of two-dimensional (2D) materials, typically with a controllable doping route for offering regular atomic arrangement as well as excellent magnetism, is crucial for both fundamental studies and spintronic applications. Here, the adsorptions of the 5f-electron actinide series (An = Ac–Am) on porous graphene-like carbon-nitride (gh-C₃N₄) layers are explored to determine their structural stabilities, electronic nature and magnetic properties using the combination of density functional theory (DFT) calculations, ab initio molecular dynamics (AIMD), Monte Carlo (MC) simulations and chemical bonding analyses. Our investigations reveal that each An atom can be individually adsorbed at the vacancy site of gh-C₃N₄ sheet with high energetic, thermal and dynamical stabilities, which are rooted in the major interactions of ionic An–N bonding as well as the minor interactions of covalent bonding of An-5f6d states with N-2s2p states. The delocalization of a very few 5f electrons is dependent on whether they occupy the suborbitals that are matching and conducive to hybridize with the ligand orbitals forming the 5f–2s2p covalent bonds. We propose that the Ruderman–Kittel–Kasuya–Yosida (RKKY) mechanism plays a determining role for the inter-atomic 5f–5f magnetic exchange via the 6d electrons as the conduction electrons. Large magnetic moment and magnetic anisotropy energy (MAE) from the localized 5f electrons, together with the metallic characteristics owing to the delocalized 6d electrons, render these An-based 2D materials excellent metallic magnets, especially for the U@gh-C₃N₄ system with the modest magnetic moment of 0.6 μ_B, large MAE of 53 meV and high Curie temperature (T_C) of 538 K.

更新日期：2023-09-30

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南