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The Journal of Physical Chemistry A

Open Quantum System Response from the Hierarchy of Pure States

Richard Hartmann, Walter T. Strunz

Published Aug 5, 2021• 11 citations
Publisher

Abstract

The spectral properties of a quantum system are essential when probing theoretical predictions against experimental data. For an open quantum system strongly interacting with its environment, spectral features are challenging to calculate. Here we demonstrate that the stochastic Hierarchy of Pure States (HOPS) approach is well suited to calculate the response of an open quantum system to a, possibly strong, coherent probe driving. For weak driving, where Kubo’s linear response theory is applicable, it turns out that the HOPS method is highly efficient since fluctuations inherent to the stochastic dynamics cancel for the response function and, thus, allow us to obtain the susceptibility easily. Our results are in agreement with experimental data for a strongly damped spin system showing that the transition from oscillatory to overdamped motion is also reflected by the transmission spectrum. As a further application we demonstrate that the susceptibility, quantifying the amplitude of the response, as a function of temperature exhibits a maximum which is the hallmark of stochastic resonance. Beyond the linear regime, the exact open system dynamics shows the asymptotic Floquet state. We use the topic of probe driving and response to present the HOPS approach in a novel and self-contained way. This includes the importance sampling scheme which yields the nonlinear HOPS as well as the stochastic treatment of a thermal initial environmental state within the zero temperature formalism. Special attention is given to the exponential representation of the algebraic Ohmic bath correlation function and the truncation condition for the hierarchy.

DOI
10.1021/acs.jpca.1c03339

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The spectral properties of a quantum system are essential when probing theoretical predictions against experimental data. For an open quantum system strongly interacting with its environment, spectral features are challenging to calculate. Here we demonstrate that the stochastic Hierarchy of Pure States (HOPS) approach is well suited to calculate the response of an open quantum system to a, possibly strong, coherent probe driving. For weak driving, where Kubo’s linear response theory is applicable, it turns out that the HOPS method is highly efficient since fluctuations inherent to the stochastic dynamics cancel for the response function and, thus, allow us to obtain the susceptibility easily. Our results are in agreement with experimental data for a strongly damped spin system showing that the transition from oscillatory to overdamped motion is also reflected by the transmission spectrum. As a further application we demonstrate that the susceptibility, quantifying the amplitude of the response, as a function of temperature exhibits a maximum which is the hallmark of stochastic resonance. Beyond the linear regime, the exact open system dynamics shows the asymptotic Floquet state. We use the topic of probe driving and response to present the HOPS approach in a novel and self-contained way. This includes the importance sampling scheme which yields the nonlinear HOPS as well as the stochastic treatment of a thermal initial environmental state within the zero temperature formalism. Special attention is given to the exponential representation of the algebraic Ohmic bath correlation function and the truncation condition for the hierarchy.
We show that the general and numerically exact Hierarchy of Pure States method (HOPS) is very well applicable to calculate the reduced dynamics of an open quantum system. In particular, we focus on environments with a sub-Ohmic spectral density (SD) resulting in an algebraic decay of the bath correlation function (BCF). The universal applicability of HOPS, reaching from weak to strong coupling for zero and nonzero temperature, is demonstrated by solving the spin-boson model for which we find perfect agreement with other methods, each one suitable for a special regime of parameters. The challenges arising in the strong coupling regime are not only reflected in the computational effort needed for the HOPS method to converge but also in the necessity for an importance sampling mechanism, accounted for by the nonlinear variant of HOPS. In order to include nonzero-temperature effects in the strong coupling regime we found that it is highly favorable for the HOPS method to use the zero-temperature BCF and include temperature via a stochastic Hermitian contribution to the system Hamiltonian.
We derive a hierarchy of stochastic evolution equations for pure states (quantum trajectories) for open quantum system dynamics with non-Markovian structured environments. This hierarchy of pure states (HOPS) is generally applicable and provides the exact reduced density operator as an ensemble average over normalized states. The corresponding nonlinear equations are presented. We demonstrate that HOPS provides an efficient theoretical tool and apply it to the spin-boson model, the calculation of absorption spectra of molecular aggregates, and energy transfer in a photosynthetic pigment-protein complex.
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.
We present a fully quantum dynamical treatment of a quantum heat engine and its baths based on the Hierarchy of Pure States (HOPS), an exact and general method for open quantum system dynamics. We show how the change of the bath energy and the interaction energy can be determined within HOPS for arbitrary coupling strength and smooth time dependence of the modulation protocol. The dynamics of all energetic contributions during the operation can be carefully examined both in its initial transient phase and, also later, in its periodic steady state. A quantum Otto engine with a qubit as an inherently nonlinear work medium is studied in a regime where the energy associated with the interaction Hamiltonian plays an important role for the global energy balance and, thus, must not be neglected when calculating its power and efficiency. We confirm that the work required to drive the coupling with the baths sensitively depends on the speed of the modulation protocol. Remarkably, departing from the conventional scheme of well-separated phases by allowing for temporal overlap, we discover that one can even gain energy from the modulation of bath interactions. We visualize these various work contributions using the analog of state change diagrams of thermodynamic cycles. We offer a concise, full presentation of HOPS with its extension to bath observables, as it serves as a universal tool for the numerically exact description of general quantum dynamical (thermodynamic) scenarios far from the weak-coupling limit.
We derive a stochastic hierarchy of matrix product states (HOMPS) for non-Markovian dynamics in an open quantum system at finite temperature, which is numerically exact and efficient. HOMPS is obtained from the recently developed stochastic hierarchy of pure states (HOPS) by expressing HOPS in terms of formal creation and annihilation operators. The resulting stochastic first-order differential equation is then formulated in terms of matrix product states and matrix product operators. In this way the exponential complexity of HOPS can be reduced to scale polynomial with the number of particles. The validity and efficiency of HOMPS is demonstrated for the spin-boson model and long chains where each site is coupled to a structured, strongly non-Markovian environment.
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.