Understanding Discrepancies of Wavefunction Theories for Large Molecules
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arXiv
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| Format: | Preprint |
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2024
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| _version_ | 1866911222169862144 |
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| author | Schäfer, Tobias Irmler, Andreas Gallo, Alejandro Grüneis, Andreas |
| author_facet | Schäfer, Tobias Irmler, Andreas Gallo, Alejandro Grüneis, Andreas |
| contents | Quantum mechanical many-electron calculations can predict properties of atoms, molecules and even complex materials. The employed computational methods play a quintessential role in many scientifically and technologically relevant research fields. However, a question of paramount importance is whether approximations aimed at reducing the computational complexity for solving the many-electron Schrödinger equation, are accurate enough. Here, we investigate recently reported discrepancies of noncovalent interaction energies for large molecules predicted by two of the most widely-trusted many-electron theories: diffusion quantum Monte Carlo and coupled-cluster theory. We are able to unequivocally pin down the source of the puzzling discrepancies and present modifications to widely-used coupled-cluster methods needed for more accurate noncovalent interaction energies of large molecules on the hundred-atom scale. This enhances the reliability of predictions from quantum mechanical many-electron theories across a wide range of critical applications, including drug design, catalysis, and the innovation of new functional materials, such as those for renewable energy technologies. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2407_01442 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Understanding Discrepancies of Wavefunction Theories for Large Molecules Schäfer, Tobias Irmler, Andreas Gallo, Alejandro Grüneis, Andreas Chemical Physics Quantum mechanical many-electron calculations can predict properties of atoms, molecules and even complex materials. The employed computational methods play a quintessential role in many scientifically and technologically relevant research fields. However, a question of paramount importance is whether approximations aimed at reducing the computational complexity for solving the many-electron Schrödinger equation, are accurate enough. Here, we investigate recently reported discrepancies of noncovalent interaction energies for large molecules predicted by two of the most widely-trusted many-electron theories: diffusion quantum Monte Carlo and coupled-cluster theory. We are able to unequivocally pin down the source of the puzzling discrepancies and present modifications to widely-used coupled-cluster methods needed for more accurate noncovalent interaction energies of large molecules on the hundred-atom scale. This enhances the reliability of predictions from quantum mechanical many-electron theories across a wide range of critical applications, including drug design, catalysis, and the innovation of new functional materials, such as those for renewable energy technologies. |
| title | Understanding Discrepancies of Wavefunction Theories for Large Molecules |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2407.01442 |