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

Fuente: arXiv
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Main Authors: Yao, Yi-Xuan, Zhang, Hao-Yue, Liu, Cheng-Ge, Chen, Rong-Hang, Ai, Qing, Nori, Franco
Format: Preprint
Published: 2026
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author Yao, Yi-Xuan
Zhang, Hao-Yue
Liu, Cheng-Ge
Chen, Rong-Hang
Ai, Qing
Nori, Franco
author_facet Yao, Yi-Xuan
Zhang, Hao-Yue
Liu, Cheng-Ge
Chen, Rong-Hang
Ai, Qing
Nori, Franco
contents 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 ${\rm Rh(CO)_2C_5H_7O_2}$ (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.
format Preprint
id arxiv_https___arxiv_org_abs_2604_25753
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Numerically-Exact Quantum-Simulation Approach for Two-Dimensional Spectroscopy of Open Quantum Systems
Yao, Yi-Xuan
Zhang, Hao-Yue
Liu, Cheng-Ge
Chen, Rong-Hang
Ai, Qing
Nori, Franco
Quantum Physics
Optics
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 ${\rm Rh(CO)_2C_5H_7O_2}$ (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.
title Numerically-Exact Quantum-Simulation Approach for Two-Dimensional Spectroscopy of Open Quantum Systems
topic Quantum Physics
Optics
url https://arxiv.org/abs/2604.25753