CAREER: Theories for Magnetic Properties of Lanthanide and Actinide Complexes

西北大学的Toru Shiozaki获得了化学理论、模型和计算方法项目的CAREER奖，他开发了新的波函数理论和高效的计算机程序，用于精确模拟镧系元素和锕系元素配合物的磁性。高级网络基础设施部门的计算和数据支持科学与工程项目为该奖项做出了部分贡献。Shiozaki小组在完全相对论狄拉克方程的基础上发展了多组态电子结构方法，以解释f元素配合物中的大自旋-轨道和自旋-自旋相互作用和准简并电子结构。这些理论被实现到高效的并行计算机程序中，实现了包含100个或更多原子的配合物的磁性质的定量模拟，如零场分裂和电子顺磁共振参数。Shiozaki小组开发的程序包BAGEL在GNU通用公共许可证下免费提供给最终用户和其他研究人员。爱因斯坦的相对论在分子系统的磁性中起着核心作用，因为磁各向异性的来源，自旋-轨道和自旋-自旋耦合，起源于相对论。在相对论的框架中，电子的行为是由所谓的狄拉克方程控制的。这项工作发展了理论、算法和计算机程序，为磁性分子的电子结构量身定制，以有效地解决狄拉克方程。在这项工作中开发的计算工具有助于合理设计磁性材料。由这项研究产生的计算机包可以免费提供给社区。

Toru Shiozaki of Northwestern University is supported by a CAREER award from the Chemical Theory, Models and Computational Methods program in the Chemistry division to develop novel wave function theories and efficient computer programs for accurately simulating magnetic properties of lanthanide and actinide complexes. The Computational and Data-Enabled Science and Engineering program in the Advanced Cyber Infrastructure division is contributing in part to this award. The Shiozaki group develops multi-configuration electronic structure methods on the basis of the fully relativistic Dirac equation to account for large spin-orbit and spin-spin interactions and quasi-degenerate electronic structure in f-element complexes. These theories are implemented into efficient parallel computer programs, realizing the quantitative simulation of magnetic properties, such as zero-field splitting and electron paramagnetic resonance parameters, of complexes containing 100 atoms or more. The program package developed by the Shiozaki group, BAGEL, is freely available under the GNU General Public License to end users and other researchers.Einstein's theory of relativity plays a central role in magnetic properties of molecular systems, because the sources of magnetic anisotropy, the spin-orbit and spin-spin couplings, originate from relativity. In the relativistic framework, the behavior of the electrons is governed by the so-called Dirac equation. This work develops theory, algorithms, and computer programs that are tailored to the electronic structure of magnetic molecules to efficiently solve the Dirac equation. The computational tools developed in this work help to rationally design magnetic materials. The computer package resulting from this research is freely available to the community.