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.

Local Disclosure of Quantum Memory in Non-Markovian Dynamics.

Non-Markovian processes may arise in physics due to memory effects of environmental degrees of freedom. For quantum non-Markovianity, it is an ongoing debate to clarify whether such memory effects have a verifiable quantum origin, or whether they might equally be modeled by a classical memory. In this contribution, we propose a criterion to test locally for a truly quantum memory. The approach is agnostic with respect to the environment, as it solely depends on the local dynamics of the system of interest. Experimental realizations are particularly easy, as only single-time measurements on the system itself have to be performed. We study memory in a variety of physically motivated examples, both for a time-discrete case, and for time-continuous dynamics. For the latter, we are able to provide an interesting class of non-Markovian master equations with classical memory that allows for a physically measurable quantum trajectory representation.

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.

Non-Markovian Quantum Dynamics in a Squeezed Reservoir.

We study non-Markovian dynamics of an open quantum system system interacting with a nonstationary squeezed bosonic reservoir. We derive exact and approximate descriptions for the open system dynamics. Focusing on the spin boson model, we compare exact dynamics with Redfield theory and a quantum optical master equation for both short and long time dynamics and in non-Markovian and Markov regimes. The squeezing of the bath results in asymptotic oscillations in the stationary state, which are captured faithfully by the Redfield master equation in the case of weak coupling. Furthermore, we find that the bath squeezing direction modifies the effective system-environment coupling strength and, thus, the strength of the dissipation.

Measured Composite Collision Models: Quantum Trajectory Purities and Channel Divisibility.

We investigate a composite quantum collision model with measurements on the memory part, which effectively probe the system. The framework allows us to adjust the measurement strength, thereby tuning the dynamical map of the system. For a two-qubit setup with a symmetric and informationally complete measurement on the memory, we study the divisibility of the resulting dynamics in dependence of the measurement strength. The measurements give rise to quantum trajectories of the system and we show that the average asymptotic purity depends on the specific form of the measurement. With the help of numerical simulations, we demonstrate that the different performance of the measurements is generic and holds for almost all interaction gates between the system and the memory in the composite collision model. The discrete model is then extended to a time-continuous limit.

Open Quantum System Response from the Hierarchy of Pure States.

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.

Dynamical Phase Transitions in Dissipative Quantum Dynamics with Quantum Optical Realization.

We study dynamical phase transitions (DPT) in the driven and damped Dicke model, realizable for example by a driven atomic ensemble collectively coupled to a damped cavity mode. These DPTs are characterized by nonanalyticities of certain observables, primarily the overlap of time evolved and initial state. Even though the dynamics is dissipative, this phenomenon occurs for a wide range of parameters and no fine-tuning is required. Focusing on the state of the "atoms" in the limit of a bad cavity, we are able to asymptotically evaluate an exact path integral representation of the relevant overlaps. The DPTs then arise by minimization of a certain action function, which is related to the large deviation theory of a classical stochastic process. Finally, we present a scheme which allows a measurement of the DPT in a cavity-QED setup.

Diffusive Limit of Non-Markovian Quantum Jumps.

We solve two long-standing problems for stochastic descriptions of open quantum system dynamics. First, we find the classical stochastic processes corresponding to non-Markovian quantum state diffusion and non-Markovian quantum jumps in projective Hilbert space. Second, we show that the diffusive limit of non-Markovian quantum jumps can be taken on the projective Hilbert space in such a way that it coincides with non-Markovian quantum state diffusion. However, the very same limit taken on the Hilbert space leads to a completely new diffusive unraveling, which we call non-Markovian quantum diffusion. Further, we expand the applicability of non-Markovian quantum jumps and non-Markovian quantum diffusion by using a kernel smoothing technique allowing a significant simplification in their use. Lastly, we demonstrate the applicability of our results by studying a driven dissipative two level atom in a non-Markovian regime using all of the three methods.

Steering Heat Engines: A Truly Quantum Maxwell Demon.

We address the question of verifying the quantumness of thermal machines. A Szilárd engine is truly quantum if its work output cannot be described by a local hidden state model, i.e., an objective local statistical ensemble. Quantumness in this scenario is revealed by a steering-type inequality which bounds the classically extractable work. A quantum Maxwell demon can violate that inequality by exploiting quantum correlations between the work medium and the thermal environment. While for a classical Szilárd engine an objective description of the medium always exists, any such description can be ruled out by a steering task in a truly quantum case.

Exact open quantum system dynamics: Optimal frequency vs time representation of bath correlations.

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.

Parametrization and Optimization of Gaussian Non-Markovian Unravelings for Open Quantum Dynamics.

We derive a family of Gaussian non-Markovian stochastic Schrödinger equations for the dynamics of open quantum systems. The different unravelings correspond to different choices of squeezed coherent states, reflecting different measurement schemes on the environment. Consequently, we are able to give a single shot measurement interpretation for the stochastic states and microscopic expressions for the noise correlations of the Gaussian process. By construction, the reduced dynamics of the open system does not depend on the squeezing parameters. They determine the non-Hermitian Gaussian correlation, a wide range of which are compatible with the Markov limit. We demonstrate the versatility of our results for quantum information tasks in the non-Markovian regime. In particular, by optimizing the squeezing parameters, we can tailor unravelings for improving entanglement bounds or for environment-assisted entanglement protection.

Stochastic Feshbach Projection for the Dynamics of Open Quantum Systems.

We present a stochastic projection formalism for the description of quantum dynamics in bosonic or spin environments. The Schrödinger equation in the coherent state representation with respect to the environmental degrees of freedom can be reformulated by employing the Feshbach partitioning technique for open quantum systems based on the introduction of suitable non-Hermitian projection operators. In this picture the reduced state of the system can be obtained as a stochastic average over pure state trajectories, for any temperature of the bath. The corresponding non-Markovian stochastic Schrödinger equations include a memory integral over the past states. In the case of harmonic environments and linear coupling the approach gives a new form of the established non-Markovian quantum state diffusion stochastic Schrödinger equation without functional derivatives. Utilizing spin coherent states, the evolution equation for spin environments resembles the bosonic case with, however, a non-Gaussian average for the reduced density operator.

Closures of the functional expansion hierarchy in the non-Markovian quantum state diffusion approach.

To find a practical scheme to numerically solve the non-Markovian Quantum State Diffusion equation (NMQSD), one often uses a functional expansion of the functional derivative that appears in the general NMQSD equation. This expansion leads to a hierarchy of coupled operators. It turned out that if one takes only the zeroth order term into account, one has a very efficient method that agrees remarkably well with the exact results for many cases of interest. We denote this approach as zeroth order functional expansion (ZOFE). In the present work, we investigate two extensions of ZOFE. Firstly, we investigate how the hierarchy converges when taking higher orders into account (which, however, leads to a fast increase in numerical size). Secondly, we demonstrate that by using a terminator that approximates the higher order contributions, one can obtain significant improvement, at hardly any additional computational cost. We carry out our investigations for the case of absorption spectra of molecular aggregates.

Non-Markovian Quantum State Diffusion for temperature-dependent linear spectra of light harvesting aggregates.

Non-Markovian Quantum State Diffusion (NMQSD) has turned out to be an efficient method to calculate excitonic properties of aggregates composed of organic chromophores, taking into account the coupling of electronic transitions to vibrational modes of the chromophores. NMQSD is an open quantum system approach that incorporates environmental degrees of freedom (the vibrations in our case) in a stochastic way. We show in this paper that for linear optical spectra (absorption, circular dichroism), no stochastics is needed, even for finite temperatures. Thus, the spectra can be obtained by propagating a single trajectory. To this end, we map a finite temperature environment to the zero temperature case using the so-called thermofield method. The resulting equations can then be solved efficiently by standard integrators.

Theoretical analysis of the relaxation dynamics in perylene bisimide dimers excited by femtosecond laser pulses.

We present a model for the relaxation dynamics in perylene bisimide dimers, which is based on ab initio electronic structure and quantum dynamics calculations including effects of dissipation. The excited-state dynamics proceeds via a mixing of electronic states of local Frenkel and charge-transfer characters, which becomes effective upon a small distortion of the dimer geometry. In this way, it is possible to explain the fast depopulation of the photoexcited state, which we characterize by femtosecond transient absorption measurements. The combined theoretical and experimental analysis hints at a trapping mechanism, which involves nonadiabatic and dissipative dynamics in an excited-state vibronic manifold and provides an atomistic picture that might prove valuable for future design of photovoltaic materials.

Quantum diffusion wave-function approach to two-dimensional vibronic spectroscopy.

We apply the quantum diffusion wavefunction approach to calculate vibronic two-dimensional (2D) spectra. As an example, we use a system consisting of two electronic states with harmonic oscillator potentials which are coupled to a bath and interact with three time-delayed laser pulses. The first- and second-order perturbative wave functions which enter into the expression for the third-order polarization are determined for a sufficient number of stochastic runs. The wave-packet approach, besides being an alternative technique to calculate the spectra, offers an intuitive insight into the dissipation dynamics and its relation to the 2D vibronic spectra.

Accounting for intra-molecular vibrational modes in open quantum system description of molecular systems.

Electronic-vibrational dynamics in molecular systems that interact with an environment involve a large number of degrees of freedom and are therefore often described by means of open quantum system approaches. A popular approach is to include only the electronic degrees of freedom into the system part and to couple these to a non-Markovian bath of harmonic vibrational modes that is characterized by a spectral density. Since this bath represents both intra-molecular and external vibrations, it is important to understand how to construct a spectral density that accounts for intra-molecular vibrational modes that couple further to other modes. Here, we address this problem by explicitly incorporating an intra-molecular vibrational mode together with the electronic degrees of freedom into the system part and using the Fano theory for a resonance coupled to a continuum to derive an "effective" bath spectral density, which describes the contribution of intra-molecular modes. We compare this effective model for the intra-molecular mode with the method of pseudomodes, a widely used approach in simulation of non-Markovian dynamics. We clarify the difference between these two approaches and demonstrate that the respective resulting dynamics and optical spectra can be very different.

Joint measurability in nonequilibrium quantum thermodynamics.

In this Letter we investigate the concept of quantum work and its measurability from the viewpoint of quantum measurement theory. Very often, quantum work and fluctuation theorems are discussed in the framework of projective two-point measurement (TPM) schemes. According to a well-known no-go theorem, there is no work observable which satisfies both (i) an average work condition and (ii) the TPM statistics for diagonal input states. Such projective measurements represent a restrictive class among all possible measurements. It is desirable, both from a theoretical and experimental point of view, to extend the scheme to the general case including suitably designed unsharp measurements. This shifts the focus to the question of what information about work and its fluctuations one is able to extract from such generalized measurements. We show that the no-go theorem no longer holds if the observables in a TPM scheme are jointly measurable for any intermediate unitary evolution. We explicitly construct a model with unsharp energy measurements and derive bounds for the visibility that ensure joint measurability. In such an unsharp scenario a single work measurement apparatus can be constructed that allows us to determine the correct average work and to obtain free energy differences with the help of a Jarzynski equality.

Quantum transport on honeycomb networks.

We study the transport properties on honeycomb networks motivated by graphene structures by using the continuous-time quantum walk (CTQW) model. For various relevant topologies we consider the average return probability and its long-time average as measures for the transport efficiency. These quantities are fully determined by the eigenvalues and the eigenvectors of the connectivity matrix of the network. For all networks derived from graphene structures we notice a nontrivial interplay between good spreading and localization effects. Flat graphene with similar number of hexagons along both directions shows a decrease in transport efficiency compared to more one-dimensional structures. This loss can be overcome by increasing the number of layers, thus creating a graphite network, but it gets less efficient when rolling up the sheets so that a nanotube structure is considered. We found peculiar results for honeycomb networks constructed from square graphene, i.e. the same number of hexagons along both directions of the graphene sheet. For these kind of networks we encounter significant differences between networks with an even or odd number of hexagons along one of the axes.

Non-markovian quantum state diffusion for absorption spectra of molecular aggregates.

In many molecular systems one encounters the situation where electronic excitations couple to a quasi-continuum of phonon modes. The interaction to that often structured continuum may be highly frequency dependent, e.g. due to some weakly damped high frequency modes. To handle such a situation, an approach combining the non-markovian quantum state diffusion description of open quantum systems with an efficient but abstract approximation was recently applied to calculate energy transfer and absorption spectra of molecular aggregates [J. Roden, A. Eisfeld, W. Wolff, W. T. Strunz, Phys. Rev. Lett. 103, 058301 (2009)]. To explore the validity of the used approximation for such complicated systems, in the present work we compare the calculated (approximative) absorption spectra with exact results. These are obtained from the method of pseudomodes, which we show to be capable of determining the exact spectra for small aggregates and a few pseudomodes. It turns out that in the cases considered, the results of the two approaches mostly agree quite well. The advantages and disadvantages of the two approaches are discussed.