Numerically-Exact Quantum-Simulation Approach for Two-Dimensional Spectroscopy of Open Quantum Systems

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 (BET), 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 (CLS) method for extracting time correlation functions (TCFs) from the 2DS. We further apply our approach to the 2DS of $\mathrm{Rh}(\mathrm{CO}{)}_2{\mathrm{C}}_5{\mathrm{H}}_7{\mathrm{O}}_2$ (RDC) 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.

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