论文标题
多配合自谐场方法中的分子磁性
Molecular magnetism in the multi-configurational self-consistent field method
论文作者
论文摘要
我们开发了我们最近文章中使用的结构化理论框架。物理。 J. B 92，93（2019）和Phys。 Rev. B 101，094427（2020）]表征了磁谱，磁化和磁敏感性的异常行为，分子磁铁Ni $ _4 $ MO $ $ $ _ {12} $。理论背景基于分子轨道理论，结合了多种配置的自洽场方法，并导致了用于构建相应能量谱的植入后循环方案。此外，我们构建了一种双线性自旋样哈密顿量，涉及离散的耦合参数，该参数涉及相关的光谱磁激发，磁化和磁敏感性。确定随后的哈密顿素化的特征力表达，并讨论了磁光谱中实验观察到的峰的拓宽和分裂的物理起源。为了证明我们方法的效率，我们计算了自旋磁二聚体的光谱特性。目前的方法可以根据过渡金属和稀土元素应用于多种磁性单元。
We develop a structured theoretical framework used in our recent articles [Eur. Phys. J. B 92, 93 (2019) and Phys. Rev. B 101, 094427 (2020)] to characterize the unusual behavior of the magnetic spectrum, magnetization and magnetic susceptibility of the molecular magnet Ni$_4$Mo$_{12}$. The theoretical background is based on the molecular orbital theory in conjunction with the multi-configurational self-consistent field method and results in a post-Hartree-Fock scheme for constructing the corresponding energy spectrum. Furthermore, we construct a bilinear spin-like Hamiltonian involving discrete coupling parameters accounting for the relevant spectroscopic magnetic excitations, magnetization and magnetic susceptibility. The explicit expressions of the eigenenergies of the ensuing Hamiltonian are determined and the physical origin of broadening and splitting of experimentally observed peaks in the magnetic spectra is discussed. To demonstrate the efficiency of our method we compute the spectral properties of a spin-one magnetic dimer. The present approach may be applied to a variety of magnetic units based on transition metals and rare earth elements.
