Simulating Non-Markovian Dynamics in Multidimensional Electronic Spectroscopy via Quantum Algorithm

TL;DR

This paper introduces a quantum algorithm for simulating non-Markovian dynamics in multidimensional electronic spectroscopy, enabling accurate modeling of complex molecular environments and their spectral responses.

Contribution

It presents a novel quantum algorithm utilizing pseudomode embedding and collision models to simulate nonlinear spectroscopy in structured environments.

Findings

Successfully simulated spectra of an excitonic dimer with different environments

Demonstrated the potential for quantum algorithms to capture spectral features like lineshape and relaxation

Validated the approach with finite-memory environment models

Abstract

Including the effect of the molecular environment in the numerical modeling of time-resolved electronic spectroscopy remains an important challenge in computational spectroscopy. In this contribution, we present a general approach for the simulation of the optical response of multi-chromophore systems in a structured environment and its implementation as a quantum algorithm. A key step of the procedure is the pseudomode embedding of the system-environment problem resulting in a finite set of quantum states evolving according to a Markovian quantum master equation. This formulation is then solved by a collision model integrated into a quantum algorithm designed to simulate linear and nonlinear response functions. The workflow is validated by simulating spectra for the prototypical excitonic dimer interacting with fast (memoryless) and finite-memory environments. The results demonstrate, on the one hand, the potential of the pseudomode embedding for simulating the dynamical features of nonlinear spectroscopy, including lineshape, spectral diffusion, and relaxations along delay times. On the other hand, the explicit synthesis of quantum circuits provides a fully quantum simulation protocol of nonlinear spectroscopy harnessing the efficient quantum simulation of many-body dynamics promised by the future generation of fault-tolerant quantum computers.