Simulating real-time molecular electron dynamics efficiently using the time-dependent density matrix renormalization group
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arXiv
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| Autores principales: | , |
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| Formato: | Preprint |
| Publicado: |
2024
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| _version_ | 1866913577644851200 |
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| author | Wahyutama, Imam S. Larsson, Henrik R. |
| author_facet | Wahyutama, Imam S. Larsson, Henrik R. |
| contents | Compared to ground state electronic structure optimizations, accurate simulations of molecular real-time electron dynamics are usually much more difficult to perform. To simulate electron dynamics, the time-dependent density matrix renormalization group (TDDMRG) has been shown to offer an attractive compromise between accuracy and cost. However, many simulation parameters significantly affect the quality and efficiency of a TDDMRG simulation. So far, it is unclear whether common wisdom from ground state DMRG carries over to the TDDMRG, and a guideline on how to choose these parameters is missing. Here, in order to establish such a guideline, we investigate the convergence behavior of the main TDDMRG simulation parameters, such as time integrator, the choice of orbitals, and the choice of matrix-product-state representation for complex-valued non-singlet states. In addition, we propose a method to select orbitals that are tailored to optimize the dynamics. Lastly, we showcase the TDDMRG by applying it to charge migration ionization dynamics in furfural, where we reveal a rapid conversion from an ionized state with a $σ$ character to one with a $π$ character within less than a femtosecond. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2409_05959 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Simulating real-time molecular electron dynamics efficiently using the time-dependent density matrix renormalization group Wahyutama, Imam S. Larsson, Henrik R. Chemical Physics Strongly Correlated Electrons Computational Physics Compared to ground state electronic structure optimizations, accurate simulations of molecular real-time electron dynamics are usually much more difficult to perform. To simulate electron dynamics, the time-dependent density matrix renormalization group (TDDMRG) has been shown to offer an attractive compromise between accuracy and cost. However, many simulation parameters significantly affect the quality and efficiency of a TDDMRG simulation. So far, it is unclear whether common wisdom from ground state DMRG carries over to the TDDMRG, and a guideline on how to choose these parameters is missing. Here, in order to establish such a guideline, we investigate the convergence behavior of the main TDDMRG simulation parameters, such as time integrator, the choice of orbitals, and the choice of matrix-product-state representation for complex-valued non-singlet states. In addition, we propose a method to select orbitals that are tailored to optimize the dynamics. Lastly, we showcase the TDDMRG by applying it to charge migration ionization dynamics in furfural, where we reveal a rapid conversion from an ionized state with a $σ$ character to one with a $π$ character within less than a femtosecond. |
| title | Simulating real-time molecular electron dynamics efficiently using the time-dependent density matrix renormalization group |
| topic | Chemical Physics Strongly Correlated Electrons Computational Physics |
| url | https://arxiv.org/abs/2409.05959 |