Efficient calculation of open quantum system dynamics and time-resolved spectroscopy with Distributed Memory HEOM (DM-HEOM)

Abstract

Time- and frequency resolved optical signals provide insights into the properties of light harvesting molecular complexes, including excitation energies, dipole strengths and orientations, as well as in the exciton energy flow through the complex. The hierarchical equations of motion (HEOM) provide a unifying theory, which allows one to study the combined effects of system-environment dissipation and non-Markovian memory without making restrictive assumptions about weak or strong couplings or separability of vibrational and electronic degrees of freedom. With increasing system size the exact solution of the open quantum system dynamics requires memory and compute resources beyond a single compute node. To overcome this barrier, we developed a scalable variant of HEOM. Our distributed memory HEOM, DM-HEOM, is a universal tool for open quantum system dynamics. It is used to accurately compute all experimentally accessible time- and frequency resolved processes in light harvesting molecular complexes with arbitrary system-environment couplings for a wide range of temperatures and complex sizes.

arXiv comment28 pages, 13 figures

References in corpus (17)

• Efficient simulation of strong system-environment interactions
• Exact dynamics of dissipative electronic systems and quantum transport: Hierarchical equations of motion approach
• Hierarchy of stochastic pure states for open quantum system dynamics
• Long-Lived Electronic Coherence in Dissipative Exciton-Dynamics of Light-Harvesting Complexes
• Non-Markovian entanglement dynamics in the presence of system-bath coherence
• Reduced hierarchical equations of motion in real and imaginary time: Correlated initial states and thermodynamic quantities
• High-performance solution of hierarchical equations of motions for studying energy-transfer in light-harvesting complexes
• Real-Time and Imaginary-Time Quantum Hierarchal Fokker-Planck Equations
• Modelling of Oscillations in Two-Dimensional Echo-Spectra of the Fenna-Matthews-Olson Complex
• Quantum Heat Current under Non-perturbative and Non-Markovian Conditions: Applications to Heat Machines
• Disentangling electronic and vibronic coherences in two-dimensional echo spectra
• Open systems with error bounds: spin boson model with spectral density variations
• Advancing hierarchical equations of motion for efficient evaluation of coherent two-dimensional spectroscopy
• Two-dimensional electronic spectra of the photosynthetic apparatus of green sulfur bacteria
• Modeling of Transient Absorption Spectra in Exciton Charge-Transfer Systems
• Exact Stochastic Unraveling of an Optical Coherence Dynamics by Cumulant Expansion
• Modelling excitonic-energy transfer in light-harvesting complexes

Cited by in corpus (19)

• Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
• QuTiP-BoFiN: A bosonic and fermionic numerical hierarchical-equations-of-motion library with applications in light-harvesting, quantum control, and single-molecule electronics
• Removing instabilities in the hierarchical equations of motion: exact and approximate projection approaches
• Tree tensor network state approach for solving hierarchical equations of motion
• Chebyshev Hierarchical Equations of Motion for Systems with Arbitrary Spectral Densities and Temperatures
• A partially linearized spin-mapping approach for simulating nonlinear optical spectra
• Stochastic Equation of Motion Approach to Fermionic Dissipative Dynamics. I. Formalism
• Machine Learning of Two-Dimensional Spectroscopic Data
• Energy flow in the Photosystem I supercomplex: comparison of approximative theories with DM-HEOM
• Spectral and thermodynamic properties of the Holstein polaron: Hierarchical equations of motion approach
• HierarchicalEOM.jl: An efficient Julia framework for hierarchical equations of motion in open quantum systems
• Systematic coarse-graining of environments for the non-perturbative simulation of open quantum systems
• Survey of the Hierarchical Equations of Motion in Tensor-Train format for non-Markovian quantum dynamics
• Efficient steady state solver for the hierarchical equations of motion approach: Formulation and application to charge transport through nanosystems
• Charge transport limited by nonlocal electron-phonon interaction. I. Hierarchical equations of motion approach
• Effect of disorder and polarization sequences on two-dimensional spectra of light harvesting complexes
• A hierarchical equations of motion (HEOM) analog for systems with delay: illustrated on inter-cavity photon propagation
• Two-dimensional electronic spectra from trajectory-based dynamics: pure-state Ehrenfest, spin-mapping, and mean classical path approaches
• Input-Output Hierarchical Equations Of Motion