Structural and electronic properties of solid molecular hydrogen from many-electron theories
Structural and electronic properties of solid molecular hydrogen from many-electron theories
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多电子理论中固体分子氢的结构和电子性质
DOI：
10.1103/physrevb.103.054111
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发表时间：
2021
影响因子：
3.7
通讯作者：
Gruneis Andreas
中科院分区：
文献类型：
--
作者：
Liao Ke;Shen Tong;Li Xin-Zheng;Alavi Ali;Gruneis Andreas
我们用精确的多电子理论研究了固体氢III相的结构和电子性质，并与最新的实验结果进行了比较。在二阶微扰理论水平上对C2/c-24晶体模拟的相III的原子结构进行了全优化，结果表明，在近似密度泛函水平上优化的结构存在H$2$键长的误差，导致计算的准粒子带隙和振动频率与实验结果有显著差异。利用最新优化的原子结构，我们研究了禁带闭合和振动频率随压力的变化。我们的发现与最近的实验观察结果很好地一致，并可能被证明有助于解决长期存在的金属化压力的实验估计之间的差异，这可能是由于不一致的压力校准造成的。
We study the structural and electronic properties of phase III of solid hydrogen using accurate many-electron theories and compare to state-of-the-art experimental findings. The atomic structures of phase III modelled by C2/c-24 crystals are fully optimized on the level of second-order perturbation theory, demonstrating that previously employed structures optimized on the level of approximate density functionals exhibit errors in the H$_2$ bond lengths that cause significant discrepancies in the computed quasi particle band gaps and vibrational frequencies compared to experiment. Using the newly optimized atomic structures, we study the band gap closure and change in vibrational frequencies as a function of pressure. Our findings are in good agreement with recent experimental observations and may prove useful in resolving long-standing discrepancies between experimental estimates of metallization pressures possibly caused by disagreeing pressure calibrations.