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

TL;DR

This paper develops a simple fourth-order Magnus expansion-based propagator for quantum dynamics in Liouville space, assesses the rotating wave approximation's accuracy, and benchmarks the method against higher-order and other algorithms.

Contribution

It introduces a new 4th order propagator in Liouville space, including commutator-free versions, and evaluates RWA validity in driven $\Lambda$-systems with open-system effects.

Findings

RWA performs well for weak and resonant fields

Errors increase with stronger and non-resonant fields

Bath presence reduces RWA errors in open systems

Abstract

A simple 4th order propagator [Ture and Jang, {\it J. Phys. Chem. A.} {\bf 128}, 2871 (2024)] based on the Magnus expansion (ME) is extended to the Liouville space for both closed-system and Lindbladian open-system quantum dynamics. For both dynamics, commutator free versions of 4th order propagators are provided as well. These propagators are then applied to the dynamics of a driven $\Lambda$-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 a quantitative information on how the RWA breaks down beyond weak field or for non-resonant cases. Major results are benchmarked against results of our 6th order ME-based propagator. We also provide numerical comparison of our algorithms with other 4th order algorithms for the $\Lambda$-system. These confirm reasonable performance of our simple propagators and the improvement gained through commutator-free expressions.