On the size and structure of helium snowballs formed around charged atoms and clusters of noble gases.

On the size and structure of helium snowballs formed around charged atoms and clusters of noble gases.
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DOI:
10.1021/jp406540p
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发表时间:
2014-09-18
期刊:
The journal of physical chemistry. A
影响因子:
--
通讯作者:
Echt O
Echt O
中科院分区:
其他
文献类型:
--
作者:
Bartl P;Leidlmair C;Denifl S;Scheier P;Echt O

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掺杂有氩、氪或氙的氦纳米液滴被电子电离并在质谱仪中进行分析。鉴定出 HenNgx+ 离子含有多达 7 个惰性气体 (Ng) 原子和数十个氦原子;质谱仪的高分辨率与先进的数据分析相结合,可以解读具有相同标称质量但不同数量的氦或 Ng 原子的同位素体的贡献,例如神奇的 He2084Kr2+ 和同量异位的非神奇的 He4184Kr+。这些离子丰度的异常表明离子特别稳定;出现了几种有趣的模式。也许最令人震惊的是 HenAr+ 的结果,它显示了含有 12、20 和 12 个氦原子的三种不同的类固体溶剂化壳层的证据。这一观察结果与只有第一个溶剂化壳是类固体的普遍观念背道而驰,但与 Galli 等人的计算一致。对于 HenNa+ [, , ] ,揭示了二十面体对称的三个壳。如果 HenArx+ (2 ≤ x ≤ 7) 离子总共包含 n + x = 19 个原子,则它们似乎特别稳定。 HenKrx+ 丰度分布的一系列异常表明,每次将氪原子添加到离子核心(从 Kr+ 到 Kr3+)时,都会将六个氦原子环插入溶剂化壳中。之前报道过 He12Kr2+ 和 He12Kr3+ 处存在强烈异常 [;等人。 , , ] 归因于污染。 HenXex+ (x ≤ 3) 的分布中仅出现轻微的局部异常。 HenKr+ 和 HenXe+ 的分布表现出惊人相似的广泛特征,而 HenAr+ 的分布则没有这些特征;差异暂时归因于这些离子的非常不同的碎裂动力学。
Helium nanodroplets doped with argon, krypton, or xenon are ionized by electrons and analyzed in a mass spectrometer. HenNgx+ ions containing up to seven noble gas (Ng) atoms and dozens of helium atoms are identified; the high resolution of the mass spectrometer combined with advanced data analysis make it possible to unscramble contributions from isotopologues that have the same nominal mass but different numbers of helium or Ng atoms, such as the magic He2084Kr2+ and the isobaric, nonmagic He4184Kr+. Anomalies in these ion abundances reveal particularly stable ions; several intriguing patterns emerge. Perhaps most astounding are the results for HenAr+, which show evidence for three distinct, solid-like solvation shells containing 12, 20, and 12 helium atoms. This observation runs counter to the common notion that only the first solvation shell is solid-like but agrees with calculations by Galli et al. for HenNa+ [, , ] that reveal three shells of icosahedral symmetry. HenArx+ (2 ≤ x ≤ 7) ions appear to be especially stable if they contain a total of n + x = 19 atoms. A sequence of anomalies in the abundance distribution of HenKrx+ suggests that rings of six helium atoms are inserted into the solvation shell each time a krypton atom is added to the ionic core, from Kr+ to Kr3+. Previously reported strong anomalies at He12Kr2+ and He12Kr3+ [; et al. , , ] are attributed to a contamination. Only minor local anomalies appear in the distributions of HenXex+ (x ≤ 3). The distributions of HenKr+ and HenXe+ show strikingly similar, broad features that are absent from the distribution of HenAr+; differences are tentatively ascribed to the very different fragmentation dynamics of these ions.
DOI: 10.1002/cphc.201200664
发表时间: 2013-01-14
期刊: Chemphyschem : a European journal of chemical physics and physical chemistry
影响因子: --
作者:
Bartl P;Leidlmair C;Denifl S;Scheier P;Echt O
通讯作者: Echt O
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影响因子: 4.3
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影响因子: 4.3
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发表时间: 2013-01-01
影响因子: 3.3
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DOI: 10.1063/1.456675
发表时间: 1989-02-01
影响因子: 4.4
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