Calculation of Positron Binding Energies and Electron–Positron Annihilation Rates for Atomic Systems with the Reduced Explicitly Correlated Hartree–Fock Method in the Nuclear–Electronic Orbital Framework

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• 作者：Kurt R. Brorsen ; Michael V. Pak ; Sharon Hammes-Schiffer
• 刊名：Journal of Physical Chemistry A
• 出版年：2017
• 出版时间：January 19, 2017
• 年：2017
• 卷：121
• 期：2
• 页码：515-522
• 全文大小：339K
• ISSN：1520-5215

文摘

Although the binding of a positron to a neutral atom has not been directly observed experimentally, high-level theoretical methods have predicted that a positron will bind to a neutral atom. In the present study, the binding energies of a positron to lithium, sodium, beryllium, and magnesium, as well as the electron–positron annihilation rates for these systems, are calculated using the reduced explicitly correlated Hartree–Fock (RXCHF) method within the nuclear–electronic orbital (NEO) framework. Due to the lack of explicit electron–positron correlation, NEO Hartree–Fock and full configuration interaction calculations with reasonable electronic and positronic basis sets do not predict positron binding to any of these atoms. In contrast, the RXCHF calculations predict positron binding energies and electron-positron annihilation rates in qualitative agreement with previous highly accurate but computationally expensive stochastic variational method calculations. These results illustrate that the RXCHF method can successfully describe the binding of a positron to a neutral species with no dipole moment. Moreover, the RXCHF method will be computationally tractable for calculating positron binding to molecular systems. The RXCHF approach offers a balance of accuracy and computational tractability for studying these types of positronic systems.