High accuracy exponential decomposition of bath correlation functions for arbitrary and structured spectral densities: Emerging methodologies and new approaches
H. Takahashi, Samuel L. Rudge, Christoph Kaspar, Michael Thoss, Raffaele Borrelli
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.
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.
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.
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.
Accurate simulations of thermalization in open quantum systems require a reliable representation of the bath correlation function (BCF). Numerical approaches, such as the hierarchical equations of motion and the pseudomode method, inherently approximate the BCF using a finite set of functions, which can impact simulation accuracy. In this work, we propose a practical and rigorous testing framework to assess the validity of approximate BCFs in open quantum dynamics simulations. Our approach employs a harmonic oscillator system, where the computed dynamics can be benchmarked against known exact solutions. To enable practical testing, we make two key methodological advancements. First, we develop numerical techniques to efficiently evaluate these exact solutions across a wide range of BCFs, ensuring broad applicability. Second, we introduce a moment-based state representation that significantly simplifies computations by exploiting the Gaussian nature of the system. Applications to a two-spin system and a transmon-resonator system demonstrate that our testing procedure provides error estimates that capture the qualitative trends observed in thermalization simulations. Using this methodology, we assess the performance of recently proposed BCF construction methods, highlighting both their strengths and a notable challenge posed by sub-Ohmic spectral densities at finite temperatures.
2024, 161, 151101]. The approach leverages a low-rank decomposition of the Fourier-transform relation connecting the bath correlation function to its spectral density. By capturing the time, frequency, and temperature dependencies encoded in the spectral density-autocorrelation function relation, our method significantly reduces the degrees of freedom required for simulating open quantum system dynamics. We benchmark our approach against existing methods and demonstrate its efficacy through applications to both simple models and a realistic electron transfer process in biological systems. Additionally, we show that this new approach can be effectively combined with the tensor-train formalism to investigate the quantum dynamics of systems interacting with complex non-Markovian environments. Finally, we provide a perspective on the selection and application of various spectral density discretization techniques.
Gaussian baths are widely used to model non-Markovian environments, yet the cost of accurate simulation at long times remains poorly understood, especially when spectral densities exhibit nonanalytic behavior as in a range of realistic models. We rigorously bound the complexity of representing bath correlation functions on a time interval [0,T] by sums of complex exponentials, as employed in recent variants of pseudomode and hierarchical equations of motion methods. These bounds make explicit the dependence on the maximal simulation time T, inverse temperature β, and the type and strength of singularities in an effective spectral density. For a broad class of spectral densities, the required number of exponentials is bounded independently of T, achieving time-uniform complexity. The T-dependence emerges only as polylogarithmic factors for spectral densities with strong singularities, such as step discontinuities and inverse power-law divergences. The temperature dependence is mild for bosonic environments and disappears entirely for fermionic environments. Thus, the true bottleneck for long-time simulation is not the simulation duration itself, but rather the presence of sharp nonanalytic features in the bath spectrum. Our results are instructive both for long-time simulation of non-Markovian open quantum systems, as well as for Markovian embeddings of classical generalized Langevin equations with memory kernels.
Two different numerically exact methods for open quantum system dynamics, the hierarchy of pure states (HOPS) method, and the multi-Davydov-Ansatz are discussed. We focus on the suitability of the underlying representations of bath correlations. While in the HOPS case the correct description of the bath correlation function (BCF) in the time domain is decisive, it turns out that a windowed Fourier transform of the BCF is an appropriate indicator of the quality of the discretization in the multi-Davydov-Ansatz. For the spin-boson model with sub-Ohmic spectral density considered here, a discretization of the spectral density based on an exponential distribution, used previously, turns out to be most favorable.