Simulating Non-Markovian Dynamics in Multidimensional Electronic Spectroscopy via Quantum Algorithm
arXiv:2409.05548 · doi:10.1021/acs.jctc.4c01204
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.
References in corpus (44)
- QuTiP 2: A Python framework for the dynamics of open quantum systems
- Measure for the Degree of Non-Markovian Behavior of Quantum Processes in Open Systems
- Environment-Assisted Quantum Walks in Photosynthetic Energy Transfer
- Toward the first quantum simulation with quantum speedup
- Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
- Simulating Physical Phenomena by Quantum Networks
- IBM Q Experience as a versatile experimental testbed for simulating open quantum systems
- Solving strongly correlated electron models on a quantum computer
- Quantum collision models: open system dynamics from repeated interactions
- Non-perturbative treatment of non-Markovian dynamics of open quantum systems
- Resource-efficient digital quantum simulation of -level systems for photonic, vibrational, and spin- Hamiltonians
- On the alternatives for bath correlators and spectral densities from mixed quantum-classical simulations
- Virtual excitations in the ultra-strongly-coupled spin-boson model: physical results from unphysical modes
- Pseudomodes as an effective description of memory: Non-Markovian dynamics of two-state systems in structured reservoirs
- Energy transfer in structured and unstructured environments: master equations beyond the Born-Markov approximations
- Collision model for non-Markovian quantum dynamics
- Quantum hardware simulating four-dimensional inelastic neutron scattering
- Composite quantum collision models
- Collision models can efficiently simulate any multipartite Markovian quantum dynamics
- Linear Response on a Quantum Computer
- Optimized auxiliary oscillators for the simulation of general open quantum systems
- Generalized theory of pseudomodes for exact descriptions of non-Markovian quantum processes
- Quantum algorithm for calculating molecular vibronic spectra
- Efficient Quantum Algorithm for Computing n-time Correlation Functions
- Quantum computation of magnon spectra
- Quantum simulation of dissipative collective effects on noisy quantum computers
- Variational Quantum Computation of Molecular Linear Response Properties on a Superconducting Quantum Processor
- Quantum computation of molecular response properties
- Mapping Electronic Decoherence Pathways in Molecules
- A quantum-classical decomposition of Gaussian quantum environments: a stochastic pseudomode model
- Predicting molecular vibronic spectra using time-domain analog quantum simulation
- Systematic coarse-graining of environments for the non-perturbative simulation of open quantum systems
- A quantum algorithm for solving open system dynamics on quantum computers using noise
- Pseudomode approach and vibronic non-Markovian phenomena in light harvesting complexes
- Calculating non-linear response functions for multi-dimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion
- Stochastic collision model approach to transport phenomena in quantum networks
- Simulating optical linear absorption for mesoscale molecular aggregates: an adaptive hierarchy of pure states approach
- Digital quantum simulation of NMR experiments
- Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach
- Strategies to simulate dephasing-assisted quantum transport on digital quantum computers
- Efficient formulation of multitime generalized quantum master equations: Taming the cost of simulating 2D spectra
- Modeling the unphysical pseudomode model with physical ensembles: simulation, mitigation, and restructuring of non-Markovian quantum noise
- Measurement of linear response functions in Nuclear Magnetic Resonance
- From Stochastic Hamiltonian to Quantum Simulation: Exploring Memory Effects in Exciton Dynamics
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