Numerically exact quantum-simulation approach for two-dimensional spectroscopy of open quantum systems
Phys. Rev. A 113, 043729 – Published 27 April, 2026
DOI: https://doi.org/10.1103/42y8-4j4g
Abstract
Two-dimensional spectroscopy (2DS) is a powerful ultrafast technique for probing electronic and vibrational dynamics in complex microscopic systems. Extracting detailed information on system dynamics and system-bath interactions from 2DS experiments requires precise theoretical simulations for comparison, which motivates the development of numerically exact and computationally efficient simulation approaches. Here, we propose a quantum-simulation approach for 2DS based on the bath-engineering technique, which has been successfully employed in quantum simulations of open quantum dynamics. To demonstrate our approach, we first simulate the 2DS of a driven four-level system in chiral enantiodetection, where we also assess the applicability of the center-line slope method for extracting time correlation functions from the 2DS. We further apply our approach to the 2DS of dissolved in chloroform, where the results reproduce the main spectral patterns observed in experiments. Our work provides a numerically exact and efficient framework for simulating 2DS, and can offer additional insight into the dynamics of open quantum systems.
