Ground-States for Metals from Converged Coupled Cluster Calculations
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arXiv
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| Format: | Preprint |
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2024
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| _version_ | 1866913635536732160 |
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| author | Schäfer, Tobias |
| author_facet | Schäfer, Tobias |
| contents | Many-electron correlation methods offer a systematic approach to predicting material properties with high precision. However, practically attaining accurate ground-state properties for bulk metals presents significant challenges. In this work, we propose a novel scheme to reach the thermodynamic limit of the total ground-state energy of metals using coupled cluster theory. We demonstrate that the coupling between long-range and short-range contributions to the correlation energy is sufficiently weak, enabling us to restrict long-range contributions to low-energy excitations in a controllable way. Leveraging this insight, we calculate the surface energy of aluminum and platinum (111), providing numerical evidence that coupled cluster theory is well-suited for modeling metallic materials, particularly in surface science. Notably, our results exhibit convergence with respect to finite-size effects, basis-set size, and coupled cluster expansion, yielding excellent agreement with experimental data. This paves the way for more efficient coupled cluster calculations for large systems and a broader utilization of the theory in realistic metallic models of materials. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2408_14237 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Ground-States for Metals from Converged Coupled Cluster Calculations Schäfer, Tobias Materials Science Chemical Physics Many-electron correlation methods offer a systematic approach to predicting material properties with high precision. However, practically attaining accurate ground-state properties for bulk metals presents significant challenges. In this work, we propose a novel scheme to reach the thermodynamic limit of the total ground-state energy of metals using coupled cluster theory. We demonstrate that the coupling between long-range and short-range contributions to the correlation energy is sufficiently weak, enabling us to restrict long-range contributions to low-energy excitations in a controllable way. Leveraging this insight, we calculate the surface energy of aluminum and platinum (111), providing numerical evidence that coupled cluster theory is well-suited for modeling metallic materials, particularly in surface science. Notably, our results exhibit convergence with respect to finite-size effects, basis-set size, and coupled cluster expansion, yielding excellent agreement with experimental data. This paves the way for more efficient coupled cluster calculations for large systems and a broader utilization of the theory in realistic metallic models of materials. |
| title | Ground-States for Metals from Converged Coupled Cluster Calculations |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2408.14237 |