Implementation of quasiclassical mapping approaches for nonadiabatic molecular dynamics in the PySurf package
Quasiclassical methods for nonadiabatic molecular dynamics, based on Mayer-Miller-Stock-Thoss mapping, are implemented in the open source computer package PySurf. This complements the implementation of surface hopping approaches performed in previous studies, and leads to a unified code that allows...
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| Main Authors: | , , , , |
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| Format: | Article (Journal) |
| Language: | English |
| Published: |
2025
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| In: |
Physical chemistry, chemical physics
Year: 2025, Volume: 27, Issue: 36, Pages: 19105-19122 |
| ISSN: | 1463-9084 |
| DOI: | 10.1039/D5CP01194A |
| Online Access: | Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1039/D5CP01194A Verlag, lizenzpflichtig, Volltext: https://pubs.rsc.org/en/content/articlelanding/2025/cp/d5cp01194a 
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| Author Notes: | David Picconi, Maximilian F. S. J. Menger, Elisa Palacino-González, Edison X. Salazar and Shirin Faraji |
| Summary: | Quasiclassical methods for nonadiabatic molecular dynamics, based on Mayer-Miller-Stock-Thoss mapping, are implemented in the open source computer package PySurf. This complements the implementation of surface hopping approaches performed in previous studies, and leads to a unified code that allows nonadiabatic dynamics simulations using various mapping approaches (Ehrenfest dynamics, the linearised semiclassical initial value representation, the Poisson-bracket mapping equation, the “unity” approach for the identity operator, the spin mapping, and the symmetrical quasiclassical windowing method) as well as different flavours of surface hopping (fewest-switches, Landau-Zener, and a mapping-inspired scheme). Furthermore, a plugin is developed to provide diabatic vibronic models as input in a sum-of-products form. This opens the way to the benchmark of different types of trajectory-based propagators on different models, against exact quantum dynamical simulations performed, e.g., by the multiconfigurational time-dependent Hartree method. Illustrative calculations, performed using the whole set of available propagators, are presented for different harmonic and anharmonic two-state models, exhibiting various degrees of correlation between vibrational modes. |
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| Item Description: | Gesehen am 09.01.2026 |
| Physical Description: | Online Resource |
| ISSN: | 1463-9084 |
| DOI: | 10.1039/D5CP01194A |