Predicted Formation of H3+ in Solid Halogen Polyhydrides at High Pressures

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• 作者：Defang Duan ; Xiaoli Huang ; Fubo Tian ; Yunxian Liu ; Da Li ; Hongyu Yu ; Bingbing Liu ; Wenjing Tian ; Tian Cui
• 刊名：Journal of Physical Chemistry A
• 出版年：2015
• 出版时间：November 12, 2015
• 年：2015
• 卷：119
• 期：45
• 页码：11059-11065
• 全文大小：472K
• ISSN：1520-5215

文摘

The structures of compressed halogen polyhydrides H_nX (X = F, Cl and n > 1) and their evolution under pressure are studied using ab initio calculation based on density functional theory. H_nF (n > 1) are metastable up to 300 GPa, whereas for H_nCl (n > 1), four new stoichiometries (H₂Cl, H₃Cl, H₅Cl, and H₇Cl) are predicted to be stable at high pressures. Interestingly, triangular H₃⁺ species are unexpectedly found in stoichiometries H₂F with [H₃]⁺[HF₂]^{鈭?/sup>, H₃F with [H₃]+[F]鈭?/sup>, H₅F with [H₃]+[HF₂]鈭?/sup>[H₂]₃, and H₅Cl with [H₃]+[Cl]鈭?/sup>[H₂] above 100 GPa. Importantly, formation processes of H₃+ species are clearly seen on the basis of comparing bond lengths, bond overlap populations, electron localization functions, and Bader charges as a functions of pressure. Further analysis reveals that the formation of H₃+ species is attributed to the pressure-induced charge transfer from hydrogen atoms to halogen atoms.}