Structural Evolution and Electronic Properties of TaSin-/0 (n=2-15) Clusters: Size-Selected Anion Photoelectron Spectroscopy and Theoretical Calculations

被引：21

作者：

Lu, Sheng-Jie ^{[1
,3
,4
]}

Xu, Hong-Guang ^{[1
,2
]}

Xu, Xi-Ling ^{[1
,2
]}

Zheng, Wei-Jun ^{[1
,2
]}

机构：

[1] Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, State Key Lab Mol React Dynam, Beijing 100190, Peoples R China

[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

[3] Heze Univ, Dept Chem & Chem Engn, Heze 274015, Shandong, Peoples R China

[4] Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China

来源：

JOURNAL OF PHYSICAL CHEMISTRY A | 2020年 / 124卷 / 47期

关键词：

TRANSITION; FILMS; ABSORPTION; SUPERATOM; ALUMINUM; SINGLES; SPECTRA; N=1-13; ATOMS; SC;

D O I：

10.1021/acs.jpca.0c09209

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The structural evolution and electronic properties of TaSin-/0 (n = 2-15) clusters are explored using anion photoelectron spectroscopy accompanied by quantum chemical calculations. The Ta atom in TaSin-/0 is inclined to interact with more Si atoms and has high coordination numbers. The theoretical calculations show that TaSi2-/0 have trianglur structures and TaSin-/0 adopt pyramid structures, while the geometries of TaSin-/0 (n = 4-7) are all exohedral structures dominated by bipyramid-based configurations with the Ta atom face-capping the Si-n motifs. TaSi8-/0 and TaSi9-10- have boat-shaped geometries, whereas TaSi9-10 neutrals adopt bipyramid-based geometries instead of boat-shaped ones. TaSi11- and TaSi12 are confirmed as the critical size of transiting from exohedral to endohedral structures for anionic and neutral clusters, respectively. TaSi12-15-/0 have pentagonal or hexagonal prism-based geometries. Natural population analysis shows that the electron transfers from Si-n skeletons to Ta atom. The second-order energy differences (Delta E-2) and incremental binding energy (Delta E-1) values exhibit strong odd-even alternations, suggesting that the TaSin-odd-/0 clusters are more stable than the adjacent TaSi(n-even)(-/0 )ones, except that TaSi12-/0 are more stable than TaSi11-/0 and TaSi13-/0.

引用

页码：9818 / 9831

页数：14

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