A simple fourth order propagator based on the Magnus expansion in the Liouville space: Application to a Λ-system and assessment of the rotating wave approximation

A simple fourth-order propagator [Ture and Jang, J. Phys. Chem. A 128, 2871 (2024)] based on the Magnus expansion is extended to the Liouville space for both closed-system and Lindbladian open-system quantum dynamics. For both dynamics, commutator free versions of fourth-order propagators are provided as well. These propagators are then applied to the dynamics of a driven Λ-system, where Lindblad terms represent the effect of a photonic bath. For both dynamics, the accuracy of the rotating wave approximation (RWA) for the matter-radiation interaction is assessed. We confirmed reasonable performance of RWA for weak and resonant fields. However, small errors appear for moderate fields and substantial errors can be found for strong fields where coherent population trapping can still be expected. We also found that the presence of bath for open-system quantum dynamics consistently reduces the errors of the RWA. These results provide quantitative information on how the RWA breaks down beyond weak field or for non-resonant cases. Major results are benchmarked against results of our sixth-order ME-based propagator. We also provide numerical comparison of our algorithms with other fourth-order algorithms for the Λ-system. These confirm reasonable performance of our simple propagators and the improvement gained through commutator-free expressions.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2026-02-06
DOI
https://doi.org/10.1063/5.0314773
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
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article

A simple fourth order propagator based on the Magnus expansion in the Liouville space: Application to a Λ-system and assessment of the rotating wave approximation

Seogjoo Jang, Taner M. Ture, Changbong Hyeon
The Journal of Chemical Physics
Spectroscopy and Quantum Chemical Studies
article

A simple fourth order propagator based on the Magnus expansion in the Liouville space: Application to a Λ-system and assessment of the rotating wave approximation

Seogjoo Jang, Taner M. Ture, Changbong Hyeon
article en

Abstract

A simple fourth-order propagator [Ture and Jang, J. Phys. Chem. A 128, 2871 (2024)] based on the Magnus expansion is extended to the Liouville space for both closed-system and Lindbladian open-system quantum dynamics. For both dynamics, commutator free versions of fourth-order propagators are provided as well. These propagators are then applied to the dynamics of a driven Λ-system, where Lindblad terms represent the effect of a photonic bath. For both dynamics, the accuracy of the rotating wave approximation (RWA) for the matter-radiation interaction is assessed. We confirmed reasonable performance of RWA for weak and resonant fields. However, small errors appear for moderate fields and substantial errors can be found for strong fields where coherent population trapping can still be expected. We also found that the presence of bath for open-system quantum dynamics consistently reduces the errors of the RWA. These results provide quantitative information on how the RWA breaks down beyond weak field or for non-resonant cases. Major results are benchmarked against results of our sixth-order ME-based propagator. We also provide numerical comparison of our algorithms with other fourth-order algorithms for the Λ-system. These confirm reasonable performance of our simple propagators and the improvement gained through commutator-free expressions.

The Journal of Chemical PhysicsVol. 164(5)
Queens College, CUNY (US), The Graduate Center, CUNY (US), Korea Institute for Advanced Study (KR)
Openalex Percentile: Top 64%
Spectroscopy and Quantum Chemical Studies
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A simple fourth order propagator based on the Magnus expansion in the Liouville space: Application to a Λ-system and assessment of the rotating wave approximation — Seogjoo Jang, Taner M. Ture, et al. · The Journal of Chemical Physics (2026) | TGRS Research Map | TGRS