Structure and Properties of Cubic PuH2 and PuH3: A Density Functional Theory Study
Structure and Properties of Cubic PuH2 and PuH3: A Density Functional Theory Study
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DOI：
10.3390/cryst12101499
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发表时间：
2022-10
期刊：
影响因子：
2.7
通讯作者：
Thomas Smith;S. Moxon;D. Cooke;Lisa J. Gillie;R. M. Harker;Mark T. Storr;E. L. da Silva;M. Molinari
中科院分区：
文献类型：
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作者：
Thomas Smith;S. Moxon;D. Cooke;Lisa J. Gillie;R. M. Harker;Mark T. Storr;E. L. da Silva;M. Molinari
由于材料的自燃性和催化Pu氧化反应形成PuO2的能力，在长期储存期间存在Pu氢腐蚀产物立方PuH2和PuH3是令人关注的。本文采用密度泛函理论（DFT）对立方相PuH2和PuH3进行了模拟，并采用格里姆D3方法对PBESol+U+SOC（0 ≤ U ≤ 7 eV）的性能（包括货车德瓦耳斯色散）和杂化HSE 06 sol + SOC的性能进行了评估，研究了立方相氢化物的结构、磁性和电子学性质.我们考虑自旋轨道耦合（SOC）和非共线磁性来研究铁磁（FM），纵向和横向反铁磁（AFM）顺序排列，和方向。混合DFT证实，FM订单和方向是最稳定的立方PuH2和PuH3，分别。对于标准DFT，最稳定的磁序取决于所使用的U值，对于PuH2和PuH3都可以看到在较高U值（U > 5 eV）处的磁序跃迁。
The presence of cubic PuH2 and PuH3, the products of hydrogen corrosion of Pu, during long-term storage is of concern because of the materials’ pyrophoricity and ability to catalyse the oxidation reaction of Pu to form PuO2. Here, we modelled cubic PuH2 and PuH3 using Density Functional Theory (DFT) and assessed the performance of the PBEsol+U+SOC (0 ≤ U ≤ 7 eV) including van der Waals dispersion using the Grimme D3 method and the hybrid HSE06sol+SOC. We investigated the structural, magnetic and electronic properties of the cubic hydride phases. We considered spin–orbit coupling (SOC) and non-collinear magnetism to study ferromagnetic (FM), longitudinal and transverse antiferromagnetic (AFM) orders aligned in the , and directions. The hybrid DFT confirmed that FM orders in the and directions were the most stable for cubic PuH2 and PuH3, respectively. For the standard DFT, the most stable magnetic order is dependent on the value of U used, with transitions in the magnetic order at higher U values (U > 5 eV) seen for both PuH2 and PuH3.