Bista Dinesh, Sengupta Turbasu, Reber Arthur C, Khanna Shiv N
Department of Physics, Virginia Commonwealth University, Richmond, VA, 23284-2000, USA.
Nanoscale. 2021 Oct 1;13(37):15763-15769. doi: 10.1039/d1nr00876e.
An isolated CoSe(PEt) cluster is non-magnetic; however, we find that a magnetic unit can be formed by fusing two CoSe(PEt) superatoms into a [CoSe(PEt)] dimer. Theoretical studies indicate that the dumbbell-shaped [CoSe(PEt)] dimer has a spin moment of 2, and the spin density is primarily localized at the interfacial Co-sites where two clusters are fused into a dimer. The dimer has a low ionization energy of 4.17 eV, allowing the dimer to donate charge to C during the formation of a cluster assembled material, as seen in recent experiments by Nuckolls and co-workers. The donation of charge causes the dimer's magnetic moment to drop from 2 to 1. We hypothesize that adding electrons to the dimer, such as doping impurities to the crystal lattice, may enhance the magnetic moment by neutralizing the charged cluster. This reveals a strategy for stabilizing magnetic moments in ligated cluster assemblies.
一个孤立的CoSe(PEt)簇是非磁性的；然而，我们发现通过将两个CoSe(PEt)超原子融合成一个[CoSe(PEt)]二聚体可以形成一个磁性单元。理论研究表明，哑铃状的[CoSe(PEt)]二聚体具有2的自旋矩，并且自旋密度主要定域在两个簇融合成二聚体的界面Co位点处。该二聚体具有4.17 eV的低电离能，这使得二聚体在形成簇组装材料的过程中能够向C提供电荷，正如Nuckolls及其同事最近的实验中所观察到的那样。电荷的提供导致二聚体的磁矩从2降至1。我们推测向二聚体添加电子，例如向晶格中掺杂杂质，可能会通过中和带电簇来增强磁矩。这揭示了一种在连接簇组装体中稳定磁矩的策略。
