A Multimode Classical Hierarchical Fokker-Planck Equations Approach to Molecular Vibrations: Simulating Two-Dimensional Spectra
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arXiv
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| _version_ | 1866917172941422592 |
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| author | Hoshino, Ryotaro Tanimura, Yoshitaka |
| author_facet | Hoshino, Ryotaro Tanimura, Yoshitaka |
| contents | The multimode Brownian model with nonlinear system-bath coupling offers a flexible framework for studying both intra- and intermolecular vibrational modes in condensed-phase molecular systems. This approach allows us to calculate linear and nonlinear spectra of molecular vibrations and to examine thermal effects-such as anharmonicity, energy relaxation, and dephasing-as reflected in the spectral peak profiles. In this study, we present a computer program based on classical hierarchical Fokker-Planck equations applied to three vibrational modes of a molecular liquid. The primary objective of developing this code was to simulate the two-dimensional correlation spectrum of the intramolecular modes of liquid water. [R. Hoshino and Y. Tanimura, J. Chem. Phys. 162, 044105 (2025)]. The code has been further refined to optimize grid selection and numerical integration routines for graphics processing units (GPUs). As a demonstration, we apply this setup to simulate three interacting modes representing intermolecular vibrations in water, and calculate the resulting two-dimensional terahertz-Raman signals. The code and example routines are available in the supplementary material. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2509_25840 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | A Multimode Classical Hierarchical Fokker-Planck Equations Approach to Molecular Vibrations: Simulating Two-Dimensional Spectra Hoshino, Ryotaro Tanimura, Yoshitaka Chemical Physics The multimode Brownian model with nonlinear system-bath coupling offers a flexible framework for studying both intra- and intermolecular vibrational modes in condensed-phase molecular systems. This approach allows us to calculate linear and nonlinear spectra of molecular vibrations and to examine thermal effects-such as anharmonicity, energy relaxation, and dephasing-as reflected in the spectral peak profiles. In this study, we present a computer program based on classical hierarchical Fokker-Planck equations applied to three vibrational modes of a molecular liquid. The primary objective of developing this code was to simulate the two-dimensional correlation spectrum of the intramolecular modes of liquid water. [R. Hoshino and Y. Tanimura, J. Chem. Phys. 162, 044105 (2025)]. The code has been further refined to optimize grid selection and numerical integration routines for graphics processing units (GPUs). As a demonstration, we apply this setup to simulate three interacting modes representing intermolecular vibrations in water, and calculate the resulting two-dimensional terahertz-Raman signals. The code and example routines are available in the supplementary material. |
| title | A Multimode Classical Hierarchical Fokker-Planck Equations Approach to Molecular Vibrations: Simulating Two-Dimensional Spectra |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2509.25840 |