Chemically Assisted Precompression of Hydrogen Molecules in Alkaline-Earth Tetrahydrides

doi:10.1021/acs.jpclett.2c02157

	Chemically Assisted Precompression of Hydrogen Molecules in Alkaline-Earth Tetrahydrides
	Pena-Alvarez, Miriam 5,6; Binns, Jack 3,4; Marques, Miriam 5,6; Kuzovnikov, Mikhail A.5,6; Dalladay-Simpson, Philip 3; Pickard, Chris J.1,7; Ackland, Graeme J.5,6; Gregoryanz, Eugene 2,3,5,6; Howie, Ross T.3,5,6
刊名	JOURNAL OF PHYSICAL CHEMISTRY LETTERS
	2022-09-15
卷号	13
ISSN号	1948-7185
DOI	10.1021/acs.jpclett.2c02157
通讯作者	Pena-Alvarez, Miriam(mpenaal@ed.ac.uk) ; Howie, Ross T.(ross.howie@ed.ac.uk)
英文摘要	Through a series of high pressure diamond anvil experiments, we report the synthesis of alkaline earth (Ca, Sr, Ba) tetrahydrides, and investigate their properties through Raman spectroscopy, X-ray diffraction, and density functional theory calculations. The tetrahydrides incorporate both atomic and quasi-molecular hydrogen, and we find that the frequency of the intramolecular stretching mode of the H(2 )units downshifts from Ca to Sr and to Ba upon compression. The experimental results indicate that the larger the host cation, the longer the H-2(delta-) bond. Analysis of the electron localization function (ELF) demonstrates that the lengthening of the H-H bond is caused by the charge transfer from the metal to H-2 and by the steric effect of the metal host on the H-H bond. This effect is most prominent for BaH4, where the precompression of H(2)(delta-)( )units at 50 GPa results in bond lengths comparable to that of pure H2 above 275 GPa.
资助项目	UKRI Future Leaders Fellowship[Mrc-Mr/T043733/1] ; European Research Council (ERC) Grant Hecate[695527] ; European Research Council (ERC) under the European Union[948895] ; National Science Foundation of China[11974034] ; National Science Foundation, Earth Sciences[EAR-1634415] ; U.S. Department of Energy[DE-FG02-94ER14466] ; U.S. Department of Energy[DE-AC02-06CH11357] ; EPSRC[EP/P020194/1] ; EPSRC[EP/T022213/1] ; UKCP consortium under the EPSRC[EP/P022561/1]
WOS关键词	SOLID HYDROGEN ; PRESSURE ; DEPENDENCE ; TRANSITION ; HYDRIDE ; VIBRON ; PHASE
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000862321000001
资助机构	UKRI Future Leaders Fellowship ; European Research Council (ERC) Grant Hecate ; European Research Council (ERC) under the European Union ; National Science Foundation of China ; National Science Foundation, Earth Sciences ; U.S. Department of Energy ; EPSRC ; UKCP consortium under the EPSRC
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/129139]
专题	中国科学院合肥物质科学研究院
通讯作者	Pena-Alvarez, Miriam; Howie, Ross T.
作者单位	1.Univ Cambridge, Dept Mat Sci & Met, Cambridge CB3 0FS, England 2.Inst Solid State Phys, Key Lab Mat Phys, Hefei 230031, Peoples R China 3.Ctr High Pressure Sci & Technol Adv Res, Shanghai 100094, Peoples R China 4.RMIT Univ, Sch Sci, Melbourne, Vic 3000, Australia 5.Univ Edinburgh, Ctr Sci Extreme Condit, Edinburgh EH9 3FD, Midlothian, Scotland 6.Univ Edinburgh, Sch Phys & Astron, Edinburgh EH9 3FD, Midlothian, Scotland 7.Tohoku Univ, Adv Inst Mat Res, Sendai, Miyagi 9808577, Japan
推荐引用方式 GB/T 7714	Pena-Alvarez, Miriam,Binns, Jack,Marques, Miriam,et al. Chemically Assisted Precompression of Hydrogen Molecules in Alkaline-Earth Tetrahydrides[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2022,13.
APA	Pena-Alvarez, Miriam.,Binns, Jack.,Marques, Miriam.,Kuzovnikov, Mikhail A..,Dalladay-Simpson, Philip.,...&Howie, Ross T..(2022).Chemically Assisted Precompression of Hydrogen Molecules in Alkaline-Earth Tetrahydrides.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,13.
MLA	Pena-Alvarez, Miriam,et al."Chemically Assisted Precompression of Hydrogen Molecules in Alkaline-Earth Tetrahydrides".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 13(2022).