利用核-电子轨道理论捕捉高压超导氢化物和冰中的核量子效应
Capturing nuclear quantum effects in high-pressure superconducting hydrides and ice with nuclear-electronic orbital theory
AI总结：
本文采用核-电子轨道密度泛函理论（NEO-DFT）方法，准确描述了高压超导氢化物和冰中的核量子效应，预测了H₃S/D₃S的氢键对称化压力以及LaH₁₀的对称结构，并成功复现了H₂O/D₂O的冰VIII到冰X相变压力。
AI中文摘要：
核量子效应对于正确描述高压下富氢材料至关重要。超导氢化物和冰是这类系统的典型例子，需要包含晶格非简谐性和核量子效应，才能正确预测和描述实验观察到的结构和相变压力。在此，我们表明核-电子轨道密度泛函理论（NEO-DFT）方法——将特定原子核与电子同等水平进行量子力学处理——能够准确描述超导氢化物和冰中的核量子效应。NEO-DFT预测了H$_3$S和D$_3$S中的氢键对称化压力，以更昂贵的随机自洽简谐近似（SSCHA）方法为基准，并在较宽的压力范围内预测了LaH$_{10}$的正确对称Fm$ar{3}$m结构。NEO-DFT还预测了H$_2$O和D$_2$O的冰VIII到冰X相变压力，与实验测量结果一致。NEO方法的准确性、计算效率和广泛适用性为对这些系统进行大规模扩展研究打开了大门。
英文摘要：
Nuclear quantum effects are essential for correctly describing hydrogen-rich materials at high pressures. Superconducting hydrides and ice are prime examples of such systems, requiring the inclusion of lattice anharmonicity and nuclear quantum effects to correctly predict and describe the structures and phase transition pressures observed experimentally. Herein, we show that the nuclear-electronic orbital density functional theory (NEO-DFT) method, which treats specified nuclei quantum mechanically on the same level as the electrons, is capable of accurately describing nuclear quantum effects in superconducting hydrides and ice. NEO-DFT predicts the hydrogen-bond symmetrization pressure in H$_3$S and D$_3$S, benchmarking against the more expensive stochastic self-consistent harmonic approximation (SSCHA) method, and predicts the correct symmetric Fm$\bar{3}$m structure for LaH$_{10}$ at a wide range of pressures. NEO-DFT also predicts the ice VIII to ice X phase transition pressures for H$_2$O and D$_2$O in agreement with experimental measurements. The accuracy, computational efficiency, and broad applicability of the NEO method opens the door for expanded large-scale studies into these types of systems.
