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

T Taner M. Ture (Department of Chemistry and Biochemistry, Queens College, City University of New York 1 , 65-30 Kissena Boulevard, Queens, New York 11367, and , New York, New York 10016,) C Changbong Hyeon (Korea Institute for Advanced Study 2 , Hoegiro 85, Dongdaemun-gu, Seoul 02455,) S Seogjoo J. Jang (Department of Chemistry and Biochemistry, Queens College, City University of New York 1 , 65-30 Kissena Boulevard, Queens, New York 11367, and , New York, New York 10016,)

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.

Article Details

Volume / Issue Vol. 164, Issue 5
Published February 07, 2026
ISSN 0021-9606
Publisher American Institute of Physics

Journal Info

The Journal of Chemical Physics

American Institute of Physics

ISSN: 0021-9606 Physical Sciences

Authors (3)

T

Taner M. Ture

Department of Chemistry and Biochemistry, Queens College, City University of New York 1 , 65-30 Kissena Boulevard, Queens, New York 11367, and , New York, New York 10016,

C

Changbong Hyeon

Korea Institute for Advanced Study 2 , Hoegiro 85, Dongdaemun-gu, Seoul 02455,

S

Seogjoo J. Jang

Department of Chemistry and Biochemistry, Queens College, City University of New York 1 , 65-30 Kissena Boulevard, Queens, New York 11367, and , New York, New York 10016,