تقرير
Nuclear-Electronic Orbital Approach to Quantization of Protons in Periodic Electronic Structure Calculations
| العنوان: | Nuclear-Electronic Orbital Approach to Quantization of Protons in Periodic Electronic Structure Calculations |
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| المؤلفون: | Xu, Jianhang, Zhou, Ruiyi, Tao, Zhen, Malbon, Christopher, Blum, Volker, Hammes-Schiffer, Sharon, Kanai, Yosuke |
| سنة النشر: | 2022 |
| مصطلحات موضوعية: | Physics - Computational Physics, Physics - Chemical Physics |
| الوصف: | The nuclear-electronic orbital (NEO) method is a well-established approach for treating nuclei quantum mechanically in molecular systems beyond the usual Born-Oppenheimer approximation. In this work, we present a strategy to implement the NEO method for periodic electronic structure calculations, particularly focused on multicomponent density functional theory (DFT). The NEO-DFT method is implemented in an all-electron electronic structure code, FHI-aims, using a combination of analytical and numerical integration techniques as well as a resolution of the identity scheme to enhance computational efficiency. After validating this implementation, proof-of-concept applications are presented to illustrate the effects of quantized protons on the physical properties of extended systems such as two-dimensional materials and liquid-semiconductor interfaces. Specifically, periodic NEO-DFT calculations are performed for a trans-polyacetylene chain, a hydrogen boride sheet, and a titanium oxide-water interface. The zero-point energy effects of the protons, as well as electron-proton correlation, are shown to noticeably impact the density of states and band structures for these systems. These developments provide a foundation for the application of multicomponent DFT to a wide range of other extended condensed matter systems. Comment: 8 figures |
| نوع الوثيقة: | Working Paper |
| DOI: | 10.1063/5.0088427 |
| URL الوصول: | http://arxiv.org/abs/2205.06328 |
| رقم الأكسشن: | edsarx.2205.06328 |
| قاعدة البيانات: | arXiv |
| DOI: | 10.1063/5.0088427 |
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