Reformulation of Time-Dependent Density Functional Theory for Non-Perturbative Dynamics: The Rabi Oscillation Problem Resolved
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arXiv
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| Format: | Preprint |
| Published: |
2024
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| _version_ | 1866914840780472320 |
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| author | Dar, Davood B. Baranova, Anna Maitra, Neepa T. |
| author_facet | Dar, Davood B. Baranova, Anna Maitra, Neepa T. |
| contents | Rabi oscillations have long been thought to be out of reach in simulations using time-dependent density functional theory (TDDFT), a prominent symptom of the failure of the adiabatic approximation for non-perturbative dynamics. We present a reformulation of TDDFT which requires response quantities only, thus enabling an adiabatic approximation to predict such dynamics accurately because the functional is evaluated on a density close to the ground-state, instead of on the fully non-perturbative density. Our reformulation applies to it any real-time dynamics, redeeming TDDFT far from equilibrium. Examples of a resonantly-driven local excitation in a model He atom, and charge-transfer in the LiCN molecule are given. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2404_14505 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Reformulation of Time-Dependent Density Functional Theory for Non-Perturbative Dynamics: The Rabi Oscillation Problem Resolved Dar, Davood B. Baranova, Anna Maitra, Neepa T. Chemical Physics Atomic Physics Computational Physics Rabi oscillations have long been thought to be out of reach in simulations using time-dependent density functional theory (TDDFT), a prominent symptom of the failure of the adiabatic approximation for non-perturbative dynamics. We present a reformulation of TDDFT which requires response quantities only, thus enabling an adiabatic approximation to predict such dynamics accurately because the functional is evaluated on a density close to the ground-state, instead of on the fully non-perturbative density. Our reformulation applies to it any real-time dynamics, redeeming TDDFT far from equilibrium. Examples of a resonantly-driven local excitation in a model He atom, and charge-transfer in the LiCN molecule are given. |
| title | Reformulation of Time-Dependent Density Functional Theory for Non-Perturbative Dynamics: The Rabi Oscillation Problem Resolved |
| topic | Chemical Physics Atomic Physics Computational Physics |
| url | https://arxiv.org/abs/2404.14505 |