论文标题
从第一原理中捕获二氧化铀的基态:晶体失真,磁性结构和声子
Capturing the ground state of uranium dioxide from first principles: crystal distortion, magnetic structure, and phonons
论文作者
论文摘要
由于自旋轨道耦合,Mott Physics,Motage Ordering和Crystal畸变之间的复杂相互作用,二氧化铀(UO $ _2 $)仍然是第一原理方法的巨大挑战。在这里,我们使用DFT+$ U $在零温度下探索UO $ _2 $,并结合上述所有现象。技术挑战是浏览DFT+$ U $生产的许多亚稳态电子状态,该国家使用$ f $ - 轨道职业矩阵控制进行搜索以搜索基态。我们将搜索限制为高对称的铁磁阶段,包括自旋轨道耦合,该耦合产生了先前未报告的职业矩阵。然后,这种新发现的职业矩阵被用作探索破碎的对称阶段的初始化。我们发现3K抗铁磁状态的氧笼与实验非常吻合,并且旋转轨道耦合和Hubbard $ u $都是关键的成分。我们证明,只有选择的声子模式对Hubbard $ u $具有很强的依赖性,而磁性订购的总体影响只有很小的影响。我们使用非弹性中子散射对声子分散曲线进行测量,我们的计算在使用$ u $的合理值时显示出良好的一致性。 DFT+$ u $的定量成功保证了对热传输和其他可观察到的理论级别的探索。
Uranium dioxide (UO$_2$) remains a formidable challenge for first-principles approaches, due to the complex interplay among spin-orbit coupling, Mott physics, magnetic ordering, and crystal distortions. Here we use DFT+$U$ to explore UO$_2$ at zero temperature, incorporating all the aforementioned phenomena. The technical challenge is to navigate the many metastable electronic states produced by DFT+$U$, which is acomplished using $f$-orbital occupation matrix control to search for the ground state. We restrict our search to the high-symmetry ferromagnetic phase, including spin-orbit coupling, which produces a previously unreported occupation matrix. This newfound occupation matrix is then used as an initialization to explore the broken symmetry phases. We find the oxygen cage distortion of the 3k antiferromagnetic state to be in excellent agreement with experiments, and both the spin-orbit coupling and the Hubbard $U$ are critical ingredients. We demonstrate that only select phonon modes have a strong dependence on the Hubbard $U$, whereas magnetic ordering has only a small influence overall. We perform measurements of the phonon dispersion curves using inelastic neutron scattering, and our calculations show good agreement when using reasonable values of $U$. The quantitative success of DFT+$U$ warrants exploration of thermal transport and other observables within this level of theory.