Recommendation of interstitial hydrogen positions in metal oxides
Recommendation of interstitial hydrogen positions in metal oxides
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金属氧化物中间隙氢位置的推荐
DOI：
10.1016/j.commatsci.2021.111068
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发表时间：
2022
影响因子：
3.3
通讯作者：
Oba Fumiyasu
中科院分区：
文献类型：
--
作者：
Tsunoda Naoki;Kumagai Yu;Oba Fumiyasu
金属氧化物中的氢杂质因其对材料性能的重要影响而成为实验和理论研究的目标。然而，氢杂质的系统模拟并不简单，因为它们显示出取决于主体氧化物的大量不同的构型，特别是在间隙位置。在这项研究中，我们利用静电势、电子局域化函数和电荷密度来推荐金属氧化物中的间隙氢位置。我们把(I)静电势的局部极小值和(Ii)电子局域化函数的局部极大值视为间隙质子中心，(Iii)电荷密度的局部极小值作为间隙氢原子和氢离子中心。通过对20种常见金属氧化物中氢杂质的第一性原理计算，我们评估了这些建议的有效性，并表明定义(I)-(III)的组合能够有效地找到最稳定的间隙组态，特别是对于质子和氢化物离子。本方法可以大大缩小间隙氢位置的搜索空间，从而降低建模氢杂质的总体计算成本。
Hydrogen impurities in metal oxides are targets of experimental and theoretical investigations because of their crucial influences on material properties. However, systematic modeling of the hydrogen impurities is not straightforward as they show a large variety of configurations depending on the host oxides, especially at interstitial sites. In this study, we utilize the electrostatic potential, electron localization function, and charge density for recommending interstitial hydrogen positions in metal oxides. We consider (i) local minima of the electrostatic potential and (ii) local maxima of the electron localization function as interstitial proton sites, and (iii) local minima of the charge density as interstitial hydrogen-atom and hydride-ion sites. We assess the validity of these recommendations using first-principles calculations for hydrogen impurities in 20 common metal oxides and show that the combination of definitions (i)–(iii) is capable of efficiently finding the most stable interstitial configurations, especially for protons and hydride ions. The present approach can substantially narrow the search space for interstitial hydrogen positions, thereby reducing the overall computational costs for modeling hydrogen impurities.