硫族铅化物阳离子低电子态的理论研究

doi:10.3866/PKU.WHXB201401023

Abstract

Abstract:

In this work, we investigate the low-lying states of PbS, PbSe, and PbTe cations based on a recently developed equation-of-motion coupled-cluster approach for ionization potentials (EOMIP-CC) with spin-orbit coupling (SOC) at the CCSD level. Equilibrium bond lengths, harmonic frequencies as well as vertical and adiabatic ionization energies are calculated with EOMIP-SOC-CCSD and reasonable agreement with available experimental data is achieved. The contribution of triples is estimated by comparing results at the CCSD(T) level with those from EOMIP-CCSD when SOC is neglected. Better agreement with experimental data can be obtained if the contribution of triples is included. According to our results, the splitting between ²Π state is larger in PbTe⁺ than that in PbS⁺ and PbSe⁺, while coupling between ²Π_1/2 and ²Σ_1/2 owing to SOC is more significant in PbS⁺ and PbSe⁺. This is because the energy difference between ²Π and ²Σ⁺ states of PbTe⁺ is larger than that in PbS⁺ and PbSe⁺ and the SOC matrix element between ²Π_1/2 and ²Σ_1/2 states in PbTe⁺ is only half those in PbS⁺ and PbSe⁺. The present work presents new estimates on properties of these low-lying states and could serve as new references for future experiments.

Key words: Spin-orbit coupling, Equation-of-motion coupled-cluster approach, Ionization energy, Lead chalcogenide

MSC2000:

O641

CAO Zhan-Li, WANG Zhi-Fan, YANG Ming-Li, WANG Fan. Theory Studies on Low-Lying States of Lead Chalcogenide Cations[J].Acta Phys. -Chim. Sin., 2014, 30(3): 431-438.

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Theory Studies on Low-Lying States of Lead Chalcogenide Cations

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