Citation: VON SZENTPÁLY László. Multiply Charged Anions, Maximum Charge Acceptance, and Higher Electron Affinities of Molecules, Superatoms, and Clusters[J]. Acta Physico-Chimica Sinica, ;2018, 34(6): 675-682. doi: 10.3866/PKU.WHXB201801021 shu

Multiply Charged Anions, Maximum Charge Acceptance, and Higher Electron Affinities of Molecules, Superatoms, and Clusters

VON SZENTPÁLY László ^,

Institut für Theoretische Chemie, Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany

Corresponding author: VON SZENTPÁLY László, lszentpaly@yahoo.com
Received Date: 30 October 2017
Revised Date: 25 December 2017
Accepted Date: 25 December 2017
Available Online: 2 June 2018

The addition of electrons to form gas-phase multiply charged anions (MCAs) normally requires sophisticated experiments or calculations.In this work, the factors stabilizing the MCAs, the maximum electron uptake of gas-phase molecules, X, and the electronic stability of MCAs X^Q^-, are discussed. The drawbacks encountered when applying computational and/or conceptual density functional theory (DFT) to MCAs are highlighted. We develop and test a different model based on the valence-state concept. As in DFT, the electronic energy, E(N, v_ex), is a continuous function of the average electron number, N, and the external potential, v_ex, of the nuclei. The valence-state-parabola is a second-order polynomial that allows extending E(N, v_ex) to dianions and higher MCAs. The model expresses the maximum electron acceptance, Q_max, and the higher electron affinities, A_Q, as simple functions of the first electron affinity, A₁, and the ionization energy, I, of the "ancestor" system. Thus, the maximum electron acceptance is Q_{max, calc} = 1 + 12A₁/7(I -A₁). The ground-state parabola model of the conceptual DFT yields approximately half of this value, and it is termed Q_{max, GS} = \begin{document}${}^{1}\!\!\diagup\!\!{}_{2}\; $\end{document} + A₁/(I -A₁). A large variety of molecules are evaluated including fullerenes, metal clusters, super-pnictogens, super-halogens (OF₃), super-alkali species (OLi₃), and neutral or charged transition-metal complexes, AB_mL_n^0/+/-. The calculated second electron affinity A_{2, calc} = A₁-(7/12)(I -A₁) is linearly correlated to the literature references A_{2, lit} with a correlation coefficient R = 0.998. A₂ or A₃ values are predicted for further 24 species. The appearance sizes, n_ap^3-, of triply charged anionic clusters and fullerenes are calculated in agreement with the literature.
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沈阳化工大学材料科学与工程学院沈阳 110142