Atomistic simulations of out-of-equilibrium quantum nuclear dynamics
Abstract The rapid advancements in ultrafast laser technology have paved the way for pumping and probing the out-of-equilibrium dynamics of nuclei in crystals. However, interpreting these experiments is extremely challenging due to the complex nonlinear responses in systems where lattice excitations...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-04-01
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| Series: | npj Computational Materials |
| Online Access: | https://doi.org/10.1038/s41524-025-01588-4 |
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| author | Francesco Libbi Anders Johansson Lorenzo Monacelli Boris Kozinsky |
| author_facet | Francesco Libbi Anders Johansson Lorenzo Monacelli Boris Kozinsky |
| author_sort | Francesco Libbi |
| collection | DOAJ |
| description | Abstract The rapid advancements in ultrafast laser technology have paved the way for pumping and probing the out-of-equilibrium dynamics of nuclei in crystals. However, interpreting these experiments is extremely challenging due to the complex nonlinear responses in systems where lattice excitations interact, particularly in crystals composed of light atoms or at low temperatures where the quantum nature of ions becomes significant. In this work, we address the nonequilibrium quantum ionic dynamics from first principles. Our approach is general and can be applied to simulate any crystal, in combination with a first-principles treatment of electrons or external machine-learning potentials. It is implemented by leveraging the nonequilibrium time-dependent self-consistent harmonic approximation (TD-SCHA), with a stable, energy-conserving, correlated stochastic integration scheme that achieves an accuracy of $${\mathcal{O}}(d{t}^{3})$$ O ( d t 3 ) . We benchmark the method with both a simple one-dimensional model to test its accuracy and a realistic 40-atom cell of SrTiO3 under THz laser pump, paving the way for simulations of ultrafast THz-Xray pump-probe spectroscopy like those performed in synchrotron facilities. |
| format | Article |
| id | doaj-art-a49f9e73e2204c4c813f2d11e59b15e0 |
| institution | Kabale University |
| issn | 2057-3960 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Computational Materials |
| spelling | doaj-art-a49f9e73e2204c4c813f2d11e59b15e02025-08-20T03:48:18ZengNature Portfolionpj Computational Materials2057-39602025-04-011111810.1038/s41524-025-01588-4Atomistic simulations of out-of-equilibrium quantum nuclear dynamicsFrancesco Libbi0Anders Johansson1Lorenzo Monacelli2Boris Kozinsky3John A. Paulson School of Engineering and Applied Sciences, Harvard UniversityJohn A. Paulson School of Engineering and Applied Sciences, Harvard UniversityDepartment of Physics, Sapienza University of RomeJohn A. Paulson School of Engineering and Applied Sciences, Harvard UniversityAbstract The rapid advancements in ultrafast laser technology have paved the way for pumping and probing the out-of-equilibrium dynamics of nuclei in crystals. However, interpreting these experiments is extremely challenging due to the complex nonlinear responses in systems where lattice excitations interact, particularly in crystals composed of light atoms or at low temperatures where the quantum nature of ions becomes significant. In this work, we address the nonequilibrium quantum ionic dynamics from first principles. Our approach is general and can be applied to simulate any crystal, in combination with a first-principles treatment of electrons or external machine-learning potentials. It is implemented by leveraging the nonequilibrium time-dependent self-consistent harmonic approximation (TD-SCHA), with a stable, energy-conserving, correlated stochastic integration scheme that achieves an accuracy of $${\mathcal{O}}(d{t}^{3})$$ O ( d t 3 ) . We benchmark the method with both a simple one-dimensional model to test its accuracy and a realistic 40-atom cell of SrTiO3 under THz laser pump, paving the way for simulations of ultrafast THz-Xray pump-probe spectroscopy like those performed in synchrotron facilities.https://doi.org/10.1038/s41524-025-01588-4 |
| spellingShingle | Francesco Libbi Anders Johansson Lorenzo Monacelli Boris Kozinsky Atomistic simulations of out-of-equilibrium quantum nuclear dynamics npj Computational Materials |
| title | Atomistic simulations of out-of-equilibrium quantum nuclear dynamics |
| title_full | Atomistic simulations of out-of-equilibrium quantum nuclear dynamics |
| title_fullStr | Atomistic simulations of out-of-equilibrium quantum nuclear dynamics |
| title_full_unstemmed | Atomistic simulations of out-of-equilibrium quantum nuclear dynamics |
| title_short | Atomistic simulations of out-of-equilibrium quantum nuclear dynamics |
| title_sort | atomistic simulations of out of equilibrium quantum nuclear dynamics |
| url | https://doi.org/10.1038/s41524-025-01588-4 |
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