Dynamics Of Open Systems Research Articles

General framework for quantifying dissipation pathways in open quantum systems. II. Numerical validation and the role of non-Markovianity.

In the previous paper [C. W. Kim and I. Franco, J. Chem. Phys. 160, 214111-1-214111-13 (2024)], we developed a theory called MQME-D, which allows us to decompose the overall energy dissipation process in open quantum system dynamics into contributions by individual components of the bath when the subsystem dynamics is governed by a Markovian quantum master equation (MQME). Here, we contrast the predictions of MQME-D against the numerically exact results obtained by combining hierarchical equations of motion (HEOM) with a recently reported protocol for monitoring the statistics of the bath. Overall, MQME-D accurately captures the contributions of specific bath components to the overall dissipation while greatly reducing the computational cost compared to exact computations using HEOM. The computations show that MQME-D exhibits errors originating from its inherent Markov approximation. We demonstrate that its accuracy can be significantly increased by incorporating non-Markovianity by exploiting time scale separations (TSS) in different components of the bath. Our work demonstrates that MQME-D combined with TSS can be reliably used to understand how energy is dissipated in realistic open quantum system dynamics.

General framework for quantifying dissipation pathways in open quantum systems. I. Theoretical formulation.

We present a general and practical theoretical framework to investigate how energy is dissipated in open quantum system dynamics. This is performed by quantifying the contributions of individual bath components to the overall dissipation of the system. The framework is based on the Nakajima-Zwanzig projection operator technique, which allows us to express the rate of energy dissipation into a specific bath degree of freedom by using traces of operator products. The approach captures system-bath interactions to all orders, but is based on second-order perturbation theory on the off-diagonal subsystem's couplings and a Markovian description of the bath. The usefulness of our theory is demonstrated by applying it to various models of open quantum systems involving harmonic oscillators or spin baths and connecting the outcomes to existing results such as our previously reported formula derived for locally coupled harmonic baths [Kim and Franco, J. Chem. Phys. 154, 084109 (2021)]. We also prove that the dissipation calculated by our theory rigorously satisfies thermodynamic principles such as energy conservation and detailed balance. Overall, the strategy can be used to develop the theory and simulation of dissipation pathways to interpret and engineer the dynamics of open quantum systems.

Decoherence rate in random Lindblad dynamics

Open quantum systems undergo decoherence, which is responsible for the transition from quantum to classical behavior. The time scale in which decoherence takes place can be analyzed using upper limits to its rate. We examine the dynamics of open chaotic quantum systems governed by random Lindblad operators sourced from Gaussian and Ginibre ensembles with Wigner-Dyson symmetry classes. In these systems, the ensemble-averaged purity decays monotonically as a function of time. This decay is governed by the decoherence rate, which is upper-bounded by the dimension of their Hilbert space and is independent of the ensemble symmetry. These findings hold upon mixing different ensembles, indicating the universal character of the decoherence rate limit. Moreover, our findings reveal that open chaotic quantum systems governed by random Lindbladians tend to exhibit the most rapid decoherence, regardless of the initial state. This phenomenon is associated with the concentration of the decoherence rate near its upper bound. Our work identifies primary features of decoherence in dissipative quantum chaos, with applications ranging from quantum foundations to high-energy physics and quantum technologies. Published by the American Physical Society 2024

Entangled two-photon quantum heat engine: Dissipative nonequilibrium dynamics and correlated statistics

Recently, the thermodynamics of open quantum systems driven by light fields has been investigated in the framework of quantum heat engines, whose output work can be measured as a spectroscopic signal. In this work, we investigate a four-level quantum heat engine that generates cascaded entangled photon pairs, treating the hot bath as an incoherent thermal pump and focusing on the correlation statistics of the output work and photon indistinguishability. We show that the dissipative nonequilibrium dynamics of this thermodynamic open quantum system can be reconstructed by correlation measurements under carefully mediated optical control. Comparing our findings with the traditional coherently pumped model, we find that the thermal pumping has the potential to generate nonclassical correlations resulting in photon indistinguishability, displaying an advantage in probing the nonequilibrium effects induced by the baths at different temperatures. Our work also demonstrates that incoherent pumping can optimize such correlations in output work beyond the classical limit. Lastly, we show that nonclassical correlations and resonant power at steady state cannot be simultaneously maximized in the weak coupling regime. Published by the American Physical Society 2024

Bexcitonics: Quasiparticle approach to open quantum dynamics.

We develop a quasiparticle approach to capture the dynamics of open quantum systems coupled to bosonic thermal baths of arbitrary complexity based on the Hierarchical Equations of Motion (HEOM). This is done by generalizing the HEOM dynamics and mapping it into that of the system in interaction with a few bosonic fictitious quasiparticles that we call bexcitons. Bexcitons arise from a decomposition of the bath correlation function into discrete features. Specifically, bexciton creation and annihilation couple the auxiliary density matrices in the HEOM. The approach provides a systematic strategy to construct exact quantum master equations that include the system-bath coupling to all orders even for non-Markovian environments. Specifically, by introducing different metrics and representations for the bexcitons it is possible to straightforwardly generate different variants of the HEOM, demonstrating that all these variants share a common underlying quasiparticle picture. Bexcitonic properties, while unphysical, offer a coarse-grained view of the correlated system-bath dynamics and its numerical convergence. For instance, we use it to analyze the instability of the HEOM when the bath is composed of underdamped oscillators and show that it leads to the creation of highly excited bexcitons. The bexcitonic picture can also be used to develop more efficient approaches to propagate the HEOM. As an example, we use the particle-like nature of the bexcitons to introduce mode-combination of bexcitons in both number and coordinate representation that uses the multi-configuration time-dependent Hartree to efficiently propagate the HEOM dynamics.

Observation of Non-Hermitian Edge Burst Effect in One-Dimensional Photonic Quantum Walk.

Non-Hermitian systems can exhibit unique quantum phases without any Hermitian counterparts. For example, the latest theoretical studies predict a new surprising phenomenon that bulk bands can localize and dissipate prominently at the system boundary, which is dubbed the non-Hermitian edge burst effect. Here we realize a one-dimensional non-Hermitian Su-Schrieffer-Heeger lattice with bulk translation symmetry implemented with a photonic quantum walk. Employing time-resolved single-photon detection to characterize the chiral motion and boundary localization of bulk bands, we determine experimentally that the dynamics underlying the non-Hermitian edge burst effect is due to the interplay of non-Hermitian skin effect and imaginary band gap closing. This new non-Hermitian physical effect deepens our understanding of quantum dynamics in open quantum systems.

Open Quantum System Dynamics from Infinite Tensor Network Contraction.

Approaching the long-time dynamics of non-Markovian open quantum systems presents a challenging task if the bath is strongly coupled. Recent proposals address this problem through a representation of the so-called process tensor in terms of a tensor network. We show that for Gaussian environments highly efficient contraction to a matrix product operator (MPO) form can be achieved with infinite MPO evolution methods, leading to significant computational speed-up over existing proposals. The result structurally resembles open system evolution with carefully designed auxiliary degrees of freedom, as in hierarchical or pseudomode methods. Here, however, these degrees of freedom are generated automatically by the MPO evolution algorithm. Moreover, the semigroup form of the resulting propagator enables us to explore steady-state physics, such as phase transitions.

Distillation of quantum non-Markovianity

Non-Markovianty of open quantum systems dynamics is a physically relevant property which is usually associated with the backflow of (quantum) information. Using this paradigmatic marker, we develop an operational framework to investigate how non-Markovianity for qubit dynamics can be distilled when many copies of the channels are used, possibly allowing for a stronger effect on the backflow of information.

A compositional account of motifs, mechanisms, and dynamics in biochemical regulatory networks

Regulatory networks depict promoting or inhibiting interactions between molecules in a biochemical system. We introduce a category-theoretic formalism for regulatory networks, using signed graphs to model the networks and signed functors to describe occurrences of one network in another, especially occurrences of network motifs. With this foundation, we establish functorial mappings between regulatory networks and other mathematical models in biochemistry. We construct a functor from reaction networks, modeled as Petri nets with signed links, to regulatory networks, enabling us to precisely define when a reaction network could be a physical mechanism underlying a regulatory network. Turning to quantitative models, we associate a regulatory network with a Lotka-Volterra system of differential equations, defining a functor from the category of signed graphs to a category of parameterized dynamical systems. We extend this result from closed to open systems, demonstrating that Lotka-Volterra dynamics respects not only inclusions and collapsings of regulatory networks, but also the process of building up complex regulatory networks by gluing together simpler pieces. Formally, we use the theory of structured cospans to produce a lax double functor from the double category of open signed graphs to that of open parameterized dynamical systems. Throughout the paper, we ground the categorical formalism in examples inspired by systems biology.

Experimental investigation of geometric quantum speed limits in an open quantum system

The quantum speed limit (QSL) is a fundamental lower bound on the evolution time for quantum systems, and its tightness has been observed to be dependent on the properties of the physical process. However, experimental studies exploring the QSL in open quantum systems are still missing. Here, we studied geometric quantum speed limits of a qubit subject to decoherence in an ensemble of chloroform molecules in a Nuclear Magnetic Resonance experiment. We controlled the system-reservoir interaction and the spin relaxation rates by adding a paramagnetic salt, allowing the observation of both Markovian and non-Markovian open system dynamics for the qubit. We used two distinguishability measures of quantum states to assess the speed of the qubit evolution: the quantum Fisher information (QFI) and Wigner-Yanase skew information (WY). For non-Markovianity and low salt concentrations, we found crossovers between QSLs related to those metrics. The WY metric sets the tighter QSL for high concentrations and Markovian dynamics. We also show that QSLs are sensitive even to small fluctuations in spin magnetization.

Transient temperature dynamics of reservoirs connected through an open quantum system.

The dynamics of open quantum systems connected with several reservoirs attract great attention due to their importance in quantum optics, biology, quantum thermodynamics, transport phenomena, etc. In many problems, the Born approximation is applicable, which implies that the influence of the open quantum system on the reservoirs can be neglected. However, in the case of long-time dynamics or mesoscopic reservoirs, the reverse influence can be crucial. In this paper, we investigate the transient dynamics of several bosonic reservoirs connected through an open quantum system. We use an adiabatic approach to study the temporal dynamics of temperatures of the reservoirs during relaxation to thermodynamic equilibrium. We show that there are various types of temperature dynamics that strongly depend on the values of dissipative rates and initial temperatures. We demonstrate that temperatures of the reservoirs, including the hottest and coldest ones, can exhibit nonmonotonic behavior. Moreover, there are moments of time during which the reservoir with an initially intermediate temperature becomes the hottest or coldest reservoir. The obtained results pave the way for managing energy flows in mesoscale and nanoscale systems.

Non-Markovian dynamics of time-fractional open quantum systems

The Time-Fractional Schrödinger Equation (TFSE) is suitable to describe the non-Markovian dynamics of a quantum system exposed to an environment, which is instructive for understanding and characterizing the time behavior of actual physical systems. Three popular TFSEs, namely Naber’s TFSE I, Naber’s TFSE II, and XGF’s TFSE, have been introduced in the form of ∂β∂tβ with β∈0,1. However, they suffer from the drawbacks. In their respective descriptions, the total probability for finding a particle in the entire space equals one only when β=1, implying that time-fractional quantum mechanics violates quantum mechanical probability conservation. By applying the three TFSEs to a basic single-qubit open system model, we discover that in describing the non-Markovian evolution of the system, the three TFSEs are limited by their own applicable ranges of β. This indicates that the three TFSEs cannot effectively describe the non-Markovian quantum dynamics. To address these issues, we introduce a well-performed TFSE by constructing a new analytic continuation of time without iβ combined with the conformable fractional derivative. In its description, for one thing, the total probability for finding the system in any single-qubit state equals one when β∈0,1. For another, the system evolves correctly in the non-Markovian manner at all values of β. Furthermore, we study the performances of the four TFSEs applying to a two-qubit open system model and show that our TFSE still possesses the above two advantages compared with the other three TFSEs.

Variational Quantum Simulation of Lindblad Dynamics via Quantum State Diffusion.

Quantum simulation of dynamics in open quantum systems is crucial but poses a significant challenge due to the non-Hermitian nature leading to nonunitary evolution and the limited quantum resources on current quantum computers. Here we introduce a variational hybrid quantum-classical algorithm designed for simulating the time evolution governed by the Lindblad master equation. Our approach involves on a stochastic unveiling of the density matrix, transforming the Lindblad equation into a wave function-based quantum state diffusion (QSD) method with the aim of reducing qubit requirements. We then apply variational quantum simulation (VQS) to efficiently capture the nonunitary evolution in QSD. We demonstrate our QSD-VQS algorithm by investigating the quantum dynamics in a two-level system subjected to an amplitude damping channel and a four-level transverse field Ising model within a dissipative environment including time-independent and periodic Hamiltonian cases. The results reveal its promising utility with upcoming hardware in the near future.

Learning Conservation Laws in Unknown Quantum Dynamics

We present a learning algorithm for discovering conservation laws given as sums of geometrically local observables in quantum dynamics. This includes conserved quantities that arise from local and global symmetries in closed and open quantum many-body systems. The algorithm combines the classical shadow formalism for estimating expectation values of observable and data analysis techniques based on singular value decompositions and robust polynomial interpolation to discover all such conservation laws in unknown quantum dynamics with rigorous performance guarantees. Our method can be directly realized in quantum experiments, which we illustrate with numerical simulations, using closed and open quantum system dynamics in a Z2 gauge theory and in many-body localized spin chains. Published by the American Physical Society 2024

Systematic Coarse Graining of Environments for the Nonperturbative Simulation of Open Quantum Systems.

Conducting precise electronic-vibrational dynamics simulations of molecular systems poses significant challenges when dealing with realistic environments composed of numerous vibrational modes. Here, we introduce a technique for the construction of effective phonon spectral densities that capture accurately open-system dynamics over a finite time interval of interest. When combined with existing nonperturbative simulation tools, our approach can reduce significantly the computational costs associated with many-body open-system dynamics.

Constant charge method or constant potential method: Which is better for molecular modeling of electrical double layers?

In molecular modeling of electrical double layers (EDLs), the constant charge method (CCM) is prized for its computational efficiency but cannot maintain electrode equipotentiality like the more resource-intensive constant potential method (CPM), potentially leading to inaccuracies. In certain scenarios, CCM can yield results identical to CPM. However, there are no clear guidelines to determine when CCM is sufficient and when CPM is required. Here, we conduct a series of molecular simulations across various electrodes and electrolytes to present a comprehensive comparison between CCM and CPM under different charging modes. Results reveal that CCM approximates CPM effectively in capturing equilibrium EDL and current-driven dynamics in open electrode systems featuring ionic liquids or regular concentration aqueous electrolytes, while CPM is indispensable in scenarios involving organic and highly concentrated aqueous electrolytes, nanoconfinement effects, and voltage-driven dynamics. This work helps to select appropriate methods for modeling EDL systems, prioritizing accuracy while considering computational efficiency.

Dynamics of a strongly coupled quantum heat engine-Computing bath observables from the hierarchy of pure states.

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.

Criteria for Davies irreducibility of Markovian quantum dynamics

The dynamics of Markovian open quantum systems are described by Lindblad master equations, generating a quantum dynamical semigroup. An important concept for such systems is (Davies) irreducibility, i.e. the question whether there exist non-trivial invariant subspaces. Steady states of irreducible systems are unique and faithful, i.e. they have full rank. In the 1970s, Frigerio showed that a system is irreducible if the Lindblad operators span a self-adjoint set with trivial commutant. We discuss a more general and powerful algebraic criterion, showing that a system is irreducible if and only if the multiplicative algebra generated by the Lindblad operators La and the operator iH+∑aLa†La , involving the Hamiltonian H, is the entire operator space. Examples for two-level systems, show that a change of Hamiltonian terms as well as the addition or removal of dissipators can render a reducible system irreducible and vice versa. Examples for many-body systems show that a large class of spin chains can be rendered irreducible by dissipators on just one or two sites. Additionally, we discuss the decisive differences between (Davies) reducibility and Evans reducibility for quantum channels and dynamical semigroups which has lead to some confusion in the recent physics literature, especially, in the context of boundary-driven systems. We give a criterion for quantum reducibility in terms of associated classical Markov processes and, lastly, discuss the relation of the main result to the stabilization of pure states and argue that systems with local Lindblad operators cannot stabilize pure Fermi-sea states.

Non-Markovian dynamics of open quantum systems via auxiliary particles with exact operator constraint

We introduce an auxiliary-particle field theory to treat the non-Markovian dynamics of driven-dissipative quantum systems of the Jaynes-Cummings type. It assigns an individual quantum field to each reservoir state and provides an analytic, faithful representation of the coupled system-bath dynamics. We apply the method to a driven-dissipative photon Bose-Einstein condensate (BEC) coupled to a reservoir of dye molecules with electronic and vibronic excitations. The complete phase diagram of this system exhibits a hidden, non-Hermitian phase transition separating temporally oscillating from biexponentially decaying photon density correlations within the BEC. On one hand, this provides a qualitative distinction of the thermal photon BEC from a laser. On the other hand, it shows that one may continuously tune from the BEC to the lasing phase by circumventing a critical point. This auxiliary-particle method is generally applicable to the dynamics of open, non-Markovian quantum systems. Published by the American Physical Society 2024

Unraveling metastable Markovian open quantum systems

We analyze the dynamics of metastable Markovian open quantum systems by unraveling their average dynamics into stochastic trajectories. We use quantum reset processes as examples to illustrate metastable phenomenology, including a simple three-state model whose metastability is of classical type, and a two-qubit model that features a metastable decoherence-free subspace. In the three-state model, the trajectories exhibit classical metastable phenomenology: fast relaxation into distinct phases and slow transitions between them. This extends the existing correspondence between classical and quantum metastability. It enables the computation of committors for the quantum phases, and the mechanisms of rare transitions between them. For the two-qubit model, the decoherence-free subspace appears in the unraveled trajectories as a slow manifold on which the quantum state has a continuous slow evolution. This provides a classical (nonmetastable) analog of this quantum effect. We discuss the general implications of these results, and we highlight the useful role of quantum reset processes for analysis of quantum trajectories in metastable systems. Published by the American Physical Society 2024