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arXiv:1904.06982 · The Journal of Chemical Physics

Chebyshev hierarchical equations of motion for systems with arbitrary spectral densities and temperatures

Hasan Rahman, Ulrich Kleinekathöfer

Published Jun 24, 2019• 39 citations
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Abstract

The time evolution in open quantum systems, such as a molecular aggregate in contact with a thermal bath, still poses a complex and challenging problem. The influence of the thermal noise can be treated using a plethora of schemes, several of which decompose the corresponding correlation functions in terms of weighted sums of exponential functions. One such scheme is based on the hierarchical equations of motion (HEOM), which is built using only certain forms of bath correlation functions. In the case where the environment is described by a complex spectral density or is at a very low temperature, approaches utilizing the exponential decomposition become very inefficient. Here, we utilize an alternative decomposition scheme for the bath correlation function based on Chebyshev polynomials and Bessel functions to derive a HEOM approach up to an arbitrary order in the environmental coupling. These hierarchical equations are similar in structure to the popular exponential HEOM scheme, but are formulated using the derivatives of the Bessel functions. The proposed scheme is tested up to the fourth order in perturbation theory for a two-level system and compared to benchmark calculations for the case of zero-temperature quantum Ohmic and super-Ohmic noise. Furthermore, the benefits and shortcomings of the present Chebyshev-based hierarchical equations are discussed.

DOI
10.1063/1.5100102

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The time evolution in open quantum systems, such as a molecular aggregate in contact with a thermal bath, still poses a complex and challenging problem. The influence of the thermal noise can be treated using a plethora of schemes, several of which decompose the corresponding correlation functions in terms of weighted sums of exponential functions. One such scheme is based on the hierarchical equations of motion (HEOM), which is built using only certain forms of bath correlation functions. In the case where the environment is described by a complex spectral density or is at a very low temperature, approaches utilizing the exponential decomposition become very inefficient. Here, we utilize an alternative decomposition scheme for the bath correlation function based on Chebyshev polynomials and Bessel functions to derive a HEOM approach up to an arbitrary order in the environmental coupling. These hierarchical equations are similar in structure to the popular exponential HEOM scheme, but are formulated using the derivatives of the Bessel functions. The proposed scheme is tested up to the fourth order in perturbation theory for a two-level system and compared to benchmark calculations for the case of zero-temperature quantum Ohmic and super-Ohmic noise. Furthermore, the benefits and shortcomings of the present Chebyshev-based hierarchical equations are discussed.
We investigated applications of the hierarchical equation of motion (HEOM) method to perform high order perturbation calculations of reduced quantum dynamics for a harmonic bath with arbitrary spectral densities. Three different schemes are used to decompose the bath spectral density into analytical forms that are suitable to the HEOM treatment: (1) The multiple Lorentzian mode model that can be obtained by numerically fitting the model spectral density. (2) The combined Debye and oscillatory Debye modes model that can be constructed by fitting the corresponding classical bath correlation function. (3) A new method that uses undamped harmonic oscillator modes explicitly in the HEOM formalism. Methods to extract system-bath correlations were investigated for the above bath decomposition schemes. We also show that HEOM in the undamped harmonic oscillator modes can give detailed information on the partial Wigner transform of the total density operator. Theoretical analysis and numerical simulations of the spin-Boson dynamics and the absorption line shape of molecular dimers show that the HEOM formalism for high order perturbations can serve as an important tool in studying the quantum dissipative dynamics in the intermediate coupling regime.
This study investigates the decomposition of bath correlation functions (BCFs) in terms of complex exponential functions, with an eye on the realistic modeling of open quantum systems based on the hierarchical equations of motion. We introduce the theoretical background of various decomposition schemes in both time and frequency domains and assess their efficiency and accuracy by demonstrating the decomposition of various BCFs. We further develop a new procedure for the decomposition of BCFs originating from highly structured spectral densities with a high accuracy and compare it with existing fitting techniques. Advantages and disadvantages of each methodology are discussed in detail with special attention to their application to the corresponding quantum dynamical problem. This work provides fundamental tools for choosing and using a variety of decomposition techniques of BCFs for the study of open quantum systems in structured environments.
The hierarchical equations of motion (HEOM) method has become one of the most popular methods for the studies of the open quantum system. However, its applicability to systems at ultra-low temperatures is largely restrained by the enormous computational cost, which is caused by the numerous exponential functions required to accurately characterize the non-Markovian memory of the reservoir environment. To overcome this problem, a Fano spectrum decomposition (FSD) scheme has been proposed recently [Cui et al., J. Chem. Phys. 151, 024110 (2019)], which expands the reservoir correlation functions using polynomial-exponential functions and hence greatly reduces the size of the memory basis set. In this work, we explicitly establish the FSD-based HEOM formalisms for both bosonic and fermionic environments. The accuracy and efficiency of the FSD-based HEOM are exemplified by the calculated low-temperature dissipative dynamics of a spin-boson model and the dynamic and static properties of a single-orbital Anderson impurity model in the Kondo regime. The encouraging numerical results highlight the practicality and usefulness of the FSD-based HEOM method for general open systems at ultra-low temperatures.
We unite two of the most widely used approaches for strongly damped, non-Markovian open quantum dynamics, the Hierarchical Equations of Motion (HEOM) and the pseudomode method by proving two statements: First, every physical bath correlation function (BCF) that can be written as a sum of NNN exponential terms can be obtained from a physical model with NNN interacting pseudomodes which are damped in Lindblad form. Second, for every such BCF there exists a non-unitary, linear transformation which mirrors the evolution of the system-pseudomode state onto the HEOM hierarchy, and vice versa. Our proofs are constructive and we give explicit expressions for the mirror transformation as well as for the pseudomode Lindbladian corresponding to a given exponential BCF. This approach also gives insight and provides elegant derivations of the corresponding Hierarchy of stochastic Pure States (HOPS) method and its nearly-unitary version, nuHOPS. Our result opens several avenues for further optimization of non-Markovian open quantum system dynamics methods.
In non-perturbative non-Markovian open quantum systems, reaching either low temperatures with the hierarchical equations of motion (HEOM) or high temperatures with the Thermalized Time Evolving Density Operator with Orthogonal Polynomials Algorithm (T-TEDOPA) formalism in Hilbert space remains challenging. We compare different ways of modeling the environment. Sampling the Fourier transform of the bath correlation function, also called temperature dependent spectral density, proves to be very effective. T-TEDOPA [Tamascelli et al., Phys. Rev. Lett. 123, 090402 (2019)] uses a linear chain of oscillators with positive and negative frequencies, while HEOM is based on the complex poles of an optimized rational decomposition of the temperature dependent spectral density [Xu et al., Phys. Rev. Lett. 129, 230601 (2022)]. Resorting to the poles of the temperature independent spectral density and of the Bose function separately is an alternative when the problem due to the huge number of Bose poles at low temperatures is circumvented. Two examples illustrate the effectiveness of the HEOM and T-TEDOPA approaches: a benchmark pure dephasing case and a two-bath model simulating the dynamics of excited electronic states coupled through a conical intersection. We show the efficiency of T-TEDOPA to simulate dynamics at a finite temperature by using either continuous spectral densities or only all the intramolecular oscillators of a linear vibronic model calibrated from ab initio data of a phenylene ethynylene dimer.
The hierarchical equations of motion (HEOM) approach is an accurate method to simulate open system quantum dynamics, which allows for systematic convergence to numerically exact results. To represent effects of the bath, the reservoir correlation functions are usually decomposed into summation of multiple exponential terms in the HEOM method. Since the reservoir correlation functions become highly non-Markovian at low temperatures or when the bath has complex band structures, a present challenge is to obtain accurate exponential decompositions that allow efficient simulation with the HEOM. In this work, we employ the barycentric representation to approximate the Fermi function and hybridization functions in the frequency domain. This method, by approximating these functions with optimized rational decomposition, greatly reduces the number of basis functions in decomposing the reservoir correlation functions, which further allows the HEOM method to be applied to ultralow temperature and general band structures. We demonstrate the efficiency, accuracy, and long-time stability of this decomposition scheme by applying it to the Anderson impurity model in the low-temperature regime with the Lorentzian and tight-binding hybridization functions.