Au3Si4- and Au4Si4: Electronically Equivalent but Different Polarity Superatoms.,The Journal of Physical Chemistry A

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Au3Si4- and Au4Si4: Electronically Equivalent but Different Polarity Superatoms.
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-08-31 , DOI: 10.1021/acs.jpca.0c05592
Kiichirou Koyasu _{1,

2} , Kazuyuki Tsuruoka ₁ , Satoshi Kameoka ₃ , An-Pang Tsai _{3,

4} , Tatsuya Tsukuda _{1,

2}

Affiliation

A series of Au_xSi₄^– cluster anions (x = 1–4) were generated most abundantly by laser ablation of a Au₄Si alloy target. Photoelectron spectroscopy and density functional theory (DFT) calculation of Au_xSi₄^– (x = 1–4) revealed that Au₃Si₄^– can be viewed as an electronically closed superatom and is composed of a Si₄ unit whose three adjacent edges of a single facet are bridged by three Au atoms. Such phase-segregated structure is facilitated by aurophilic interaction between the three Au atoms and results in a large permanent dipole moment (4.43 D). DFT calculations on an electronically equivalent superatom Au₄Si₄ predicted a new structure in which the uncoordinated Si atom of Au₃Si₄^– is bonded by Au⁺. This Au₄Si₄ is much more stable than a cubic structure previously reported and has a large HOMO–LUMO gap (1.68 eV) and a small permanent dipole moment (0.41 D).

中文翻译：

Au3Si4-和Au4Si4：电子等效但极性不同的超级原子。

一系列的Au _X的Si ₄^-簇阴离子（X = 1-4）由Au构成激光烧蚀产生最丰富₄ Si合金靶。Au _x Si ₄^–（x = 1-4）的光电子能谱和密度泛函理论（DFT）计算表明，Au ₃ Si ₄^–可以看作是一种电子闭合的超原子，由Si ₄组成单面的三个相邻边由三个Au原子桥接的单元。三个Au原子之间的亲油相互作用促进了这种相分离的结构，并导致大的永久偶极矩（4.43 D）。上的电子等效超原子DFT计算的Au ₄的Si ₄预测，其中Au构成的不协调的Si原子的新的结构₃的Si ₄^-通过金接合⁺。该Au ₄ Si ₄比先前报道的立方结构稳定得多，并且具有较大的HOMO-LUMO间隙（1.68 eV）和较小的永久偶极矩（0.41 D）。

更新日期：2020-09-24

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