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| Main Authors: | , |
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| Format: | Preprint |
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2026
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| Online Access: | https://arxiv.org/abs/2601.16913 |
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| _version_ | 1866917219655483392 |
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| author | Sha, Mo Gu, Bing |
| author_facet | Sha, Mo Gu, Bing |
| contents | Quantum geometrical molecular dynamics provides a quantum geometric picture for understanding reactive dynamics, especially excited-state conical intersection dynamics, and also a numerically exact method for strongly correlated electron-nuclear dynamics. However, there are substantial challenges in describing medium-sized molecules with tens of nuclear degrees of freedom. The main challenge is that it uses a discrete variable representation to discretize the molecular configuration space, and thus requires a tremendous number of quantum chemistry calculations to construct the electronic overlap matrix. Moreover, the expansion coefficients scale exponentially with molecular size for direct-product basis sets. We address these challenges by first introducing a coarse-grained local diabatic ansatz, followed by a tensor network representation of the expansion coefficients and the molecular time-evolution operator. With a full 24-dimensional demonstration using the pyrazine molecule, we show that such developments provide a highly accurate and computationally tractable method for high-dimensional, fully quantum, strongly coupled electron-nuclear dynamics from first principles. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2601_16913 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Coarse-Grained Geometric Quantum Dynamics in the Tensor Network Representation Sha, Mo Gu, Bing Chemical Physics Quantum geometrical molecular dynamics provides a quantum geometric picture for understanding reactive dynamics, especially excited-state conical intersection dynamics, and also a numerically exact method for strongly correlated electron-nuclear dynamics. However, there are substantial challenges in describing medium-sized molecules with tens of nuclear degrees of freedom. The main challenge is that it uses a discrete variable representation to discretize the molecular configuration space, and thus requires a tremendous number of quantum chemistry calculations to construct the electronic overlap matrix. Moreover, the expansion coefficients scale exponentially with molecular size for direct-product basis sets. We address these challenges by first introducing a coarse-grained local diabatic ansatz, followed by a tensor network representation of the expansion coefficients and the molecular time-evolution operator. With a full 24-dimensional demonstration using the pyrazine molecule, we show that such developments provide a highly accurate and computationally tractable method for high-dimensional, fully quantum, strongly coupled electron-nuclear dynamics from first principles. |
| title | Coarse-Grained Geometric Quantum Dynamics in the Tensor Network Representation |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2601.16913 |