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arXiv:2212.06099 · The Journal of Chemical Physics

Efficient simulation of open quantum systems coupled to a reservoir through multiple channels

Hanggai Nuomin, Jiaxi Wu, Peng Zhang, David N. Beratan

Published Sep 26, 2024• 2 citations
arXivHTMLPDF

Abstract

It is challenging to simulate open quantum systems that are connected to a reservoir through multiple channels. For example, vibrations may induce fluctuations in both energy gaps and electronic couplings, which represent two independent channels of system-bath couplings. Systems of this kind are ubiquitous in the processes of excited state radiationless decay. Combined with density matrix renormalization group (DMRG) and matrix product states (MPS) methods, we develop an interaction-picture chain mapping strategy for vibrational reservoirs to simulate the dynamics of these open systems, resulting in time-dependent spatially local system-bath couplings in the chain-mapped Hamiltonian. This transformation causes the entanglement generated by the system-bath interactions to be restricted within a narrow frequency window of vibrational modes, enabling efficient DMRG/MPS dynamical simulations. We demonstrate the utility of this approach by simulating singlet fission dynamics using a generalized spin-boson Hamiltonian with both diagonal and off-diagonal system-bath couplings. This approach generalizes an earlier interaction-picture chain mapping scheme, allowing for efficient and exact simulation of systems with multi-channel system-bath couplings using matrix product states, which may further our understanding of nonlocal exciton-phonon couplings in exciton transport and the non-Condon effect in energy and electron transfer.

DOI
10.1063/5.0226183

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It is challenging to simulate open quantum systems that are connected to a reservoir through multiple channels. For example, vibrations may induce fluctuations in both energy gaps and electronic couplings, which represent two independent channels of system-bath couplings. Systems of this kind are ubiquitous in the processes of excited state radiationless decay. Combined with density matrix renormalization group (DMRG) and matrix product states (MPS) methods, we develop an interaction-picture chain mapping strategy for vibrational reservoirs to simulate the dynamics of these open systems, resulting in time-dependent spatially local system-bath couplings in the chain-mapped Hamiltonian. This transformation causes the entanglement generated by the system-bath interactions to be restricted within a narrow frequency window of vibrational modes, enabling efficient DMRG/MPS dynamical simulations. We demonstrate the utility of this approach by simulating singlet fission dynamics using a generalized spin-boson Hamiltonian with both diagonal and off-diagonal system-bath couplings. This approach generalizes an earlier interaction-picture chain mapping scheme, allowing for efficient and exact simulation of systems with multi-channel system-bath couplings using matrix product states, which may further our understanding of nonlocal exciton-phonon couplings in exciton transport and the non-Condon effect in energy and electron transfer.
Modeling open quantum systems---quantum systems coupled to a bath---is of value in condensed-matter theory, cavity quantum electrodynamics, nanosciences, and biophysics. The real-time simulation of open quantum systems was advanced significantly by the recent development of chain mapping techniques and the use of matrix product states that exploit the intrinsic entanglement structure in open quantum systems. The computational cost of simulating open quantum systems, however, remains high when the bath is excited to high-lying quantum states. We develop an approach to reduce the computational costs in such cases. The interaction representation for the open quantum system is used to distribute excitations among the bath degrees of freedom so that the occupation of each bath oscillator is ensured to be low. The interaction picture also causes the matrix dimensions to be much smaller in a matrix product state of a chain-mapped open quantum system than in the Schr\"odinger picture. Using the interaction representation accelerates the calculations by one to two orders of magnitude over the existing matrix-product-state method. In the regime of strong system-bath coupling and high temperatures, the speedup can be as large as three orders of magnitude. The approach developed here is especially promising to simulate the dynamics of open quantum systems in high-temperature and strong-coupling regimes.
Modeling open quantum systems -- quantum systems coupled to a bath -- is of value in condensed matter theory, cavity quantum electrodynamics, nanosciences and biophysics. The real-time simulation of open quantum systems was advanced significantly by the recent development of chain mapping techniques and the use of matrix product states that exploit the intrinsic entanglement structure in open quantum systems. The computational cost of simulating open quantum systems, however, remains high when the bath is excited to high-lying quantum states. We develop an approach to reduce the computational costs in such cases. The interaction representation for the open quantum system is used to distribute excitations among the bath degrees of freedom so that the occupation of each bath oscillator is ensured to be low. The interaction picture also causes the matrix dimensions to be much smaller in a matrix product state of a chain-mapped open quantum system than in the Schr\odinger picture. Using the interaction representation accelerates the calculations by 1-2 orders of magnitude over existing matrix-product-state method. In the regime of strong system-bath coupling and high temperatures, the speedup can be as large as 3 orders of magnitude. The approach developed here is especially promising to simulate the dynamics of open quantum systems in the high-temperature and strong-coupling regimes.
Quantum dynamics (QD) simulation is a powerful tool for interpreting ultrafast spectroscopy experiments and unraveling their microscopic mechanism in out-of-equilibrium excited state behaviors in various chemical, biological, and material systems. Although state-of-the-art numerical QD approaches such as the time-dependent density matrix renormalization group (TD-DMRG) already greatly extended the solvable system size of general linearly coupled exciton-phonon models with up to a few hundred phonon modes, the accurate simulation of larger system sizes or strong system-environment interactions is still computationally highly challenging. Based on quantum information theory (QIT), in this work, we realize that only a small number of effective phonon modes couple to the excitonic system directly regardless of a large or even infinite number of modes in the condensed phase environment. On top of the identified small number of direct effective modes, we propose a hierarchical mapping (HM) approach through performing block Lanczos transformations on the remaining indirect modes, which transforms the Hamiltonian matrix to a nearly block-tridiagonal form and eliminates the long-range interactions. Numerical tests on model spin-boson systems and realistic singlet fission models in a rubrene crystal environment with up to 7000 modes and strong system-environment interactions indicate HM can reduce the system size by 1-2 orders of magnitude and accelerate the calculation by ∼80% without losing accuracy.
Electronic and/or vibronic coherence has been found by recent ultrafast spectroscopy experiments in many chemical, biological, and material systems. This indicates that there are strong and complicated interactions between electronic states and vibration modes in realistic chemical systems. Therefore, simulations of quantum dynamics with a large number of electronic and vibrational degrees of freedom are highly desirable. Due to the efficient compression and localized representation of quantum states in the matrix-product state (MPS) formulation, time-evolution methods based on the MPS framework, which we summarily refer to as tDMRG (time-dependent density-matrix renormalization group) methods, are considered to be promising candidates to study the quantum dynamics of realistic chemical systems. In this work, we benchmark the performances of four different tDMRG methods, including global Taylor, global Krylov, and local one-site and two-site time-dependent variational principles (1TDVP and 2TDVP), with a comparison to multiconfiguration time-dependent Hartree and experimental results. Two typical chemical systems of internal conversion and singlet fission are investigated: one containing strong and high-order local and nonlocal electron-vibration couplings and the other exhibiting a continuous phonon bath. The comparison shows that the tDMRG methods (particularly, the 2TDVP method) can describe the full quantum dynamics in large chemical systems accurately and efficiently. Several key parameters in the tDMRG calculation including the truncation error threshold, time interval, and ordering of local sites were also investigated to strike the balance between efficiency and accuracy of results.
Dynamics of open quantum systems with structured reservoirs can often be simulated efficiently with tensor network influence functionals. The standard variants of the time-evolving matrix product operator (TEMPO) method are applicable when the systems is coupled to Gaussian bosonic baths via hermitian coupling operators that mutually commute. In this work we introduce a generalization to cases where the system is coupled to a single reservoir through multiple non-commuting operators, representing the most general form of linear system-bath coupling. We construct a Gaussian influence functional that properly handles Trotter errors arising from a finite evolution time step, thus ensuring convergence for long evolution times. Based on this result, the uniform TEMPO scheme can be employed to obtain a matrix product operator form of the influence functional, enabling efficient simulations of the real-time dynamics of the open system. As a demonstration, we simulate the time evolution of driven two-level emitters coupled to a bosonic lattice at different lattice sites.
We develop a powerful tree tensor network states method that is capable of simulating exciton-phonon quantum dynamics of larger molecular complexes and open quantum systems with multiple bosonic environments. We interface this method with ab initio density functional theory to study singlet exciton fission (SF) in a pentacene dimer. With access to the full vibronic many-body wave function, we track and assign the contributions of different symmetry classes of vibrations to SF and derive energy surfaces, enabling us to dissect, understand, and describe the strongly coupled electronic and vibrational dynamics, relaxation, and reduced state cooling. This directly exposes the rich possibilities of exploiting the functional interplay of molecular symmetry, electronic structure and vibrational dynamics in SF material design. The described method can be similarly applied to other complex (bio-) molecular systems, characterised by a rich manifold of electronic states and vibronic coupling driving non-adiabatic dynamics.