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Promethium-doped silicon clusters PmSi n (n = 3–10) and their anions: structures, thermochemistry, electron affinities and magnetic moments

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Abstract

The equilibrium geometries, electronic structures and electronic properties of PmSi n (n = 3–10) clusters were systematically investigated using the ABCluster global search technique combined with density functional methods. The results revealed that the most stable structure of neutral PmSi n and their anions can be viewed as replacing a Si atom of the ground state structure of Si n+1 with a Pm atom. The adiabatic electron affinities of PmSi n are evaluated, and they differ little from those of SmSi n and EuSi n . Analyses of HOMO–LUMO gaps showed that introducing Pm atom to Si cluster can significantly improve photochemical reactivity of the cluster. And the improved effects are as good as those of the introducing Sm and Eu atom to Si cluster. The NPA calculations indicated that the 4f electrons of Pm atom in PmSi n (n = 3–10) clusters hardly participate in bonding and provide the total magnetic moments. Dissociation energy (DE) of rare earth metal (REM) atom from the lowest energy structure of REMSi n (n = 3–10) and their anions was calculated. The DEs of PmSi n , SmSi n and EuSi n are nearly identical. The DEs of PmSi − n , SmSi − n and EuSi − n are also nearly equal, and they are smaller than those of HoSi − n and PrSi − n .

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Acknowledgements

This study was supported by the National Natural Science Foundation of China (Grant No. 21263010), by Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region (Gran No. NMGIRT-A1603), by the Inner Mongolia Natural Science Foundation (Grant No. 2015MS0216), and by the Inner Mongolia institutions of higher learning scientific research projects (Grant No. NJZY16419).

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Authors and Affiliations

  1. School of Chemical Engineering, Inner Mongolia University of Technology and Inner Mongolia Key Laboratory of Theoretical and Computational Chemistry Simulation, Hohhot, 010051, People’s Republic of China

    Shuang He & Jucai Yang

  2. Inner Mongolia Vocational College of Chemical Engineering, Hohhot, 010070, People’s Republic of China

    Shuang He

  3. School of Energy and Power Engineering, Inner Mongolia University of Technology, Hohhot, 010051, People’s Republic of China

    Jucai Yang

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Correspondence to Jucai Yang.

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He, S., Yang, J. Promethium-doped silicon clusters PmSi n (n = 3–10) and their anions: structures, thermochemistry, electron affinities and magnetic moments. Theor Chem Acc 136, 93 (2017). https://doi.org/10.1007/s00214-017-2126-7

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