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The Journal of Physical Chemistry Letters

Recovery of Purity in Dissipative Tunneling Dynamics

Sambarta Chatterjee, Nancy Makri

Published Sep 25, 2020• 13 citations
Publisher

Abstract

The time evolution of purity for an initially localized state of a symmetric two-level system coupled to a dissipative bath is investigated using numerically exact real-time path integral methods. With strong system-bath coupling and high temperature, the purity decays monotonically to its fully mixed value, with a short-time Gaussian behavior, which is subsequently followed by exponential evolution. However, under low-temperature and weak coupling conditions, a substantial recovery of purity is observed. A simple theoretical analysis reveals three contributions that correspond to a completely incoherent, eigenstate population difference and rate terms. The last two of these terms can counter the early drop of purity and are responsible for its rebound. These findings caution against using purity as a measure of decoherence in the dynamics of quantum dissipative systems.

DOI
10.1021/acs.jpclett.0c02513

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•Jan 1, 2021•0 citations
The time evolution of purity for an initially localized state of a symmetric two-level system coupled to a dissipative bath is investigated using numerically exact real-time path integral methods. With strong system-bath coupling and high temperature, the purity decays monotonically to its fully mixed value, with a short-time Gaussian behavior, which is subsequently followed by exponential evolution. However, under low-temperature and weak coupling conditions, a substantial recovery of purity is observed. A simple theoretical analysis reveals three contributions that correspond to a completely incoherent, eigenstate population difference and rate terms. The last two of these terms can counter the early drop of purity and are responsible for its rebound. These findings caution against using purity as a measure of decoherence in the dynamics of quantum dissipative systems.
The time evolution of the purity (the trace of the square of the reduced density matrix) and von Neumann entropy in a symmetric two-level system coupled to a dissipative harmonic bath is investigated through analytical arguments and accurate path integral calculations on simple models and the singly excited bacteriochlorophyll dimer. A simple theoretical analysis establishes bounds and limiting behaviors. The contributions to purity from a purely incoherent term obtained from the diagonal elements of the reduced density matrix, a term associated with the difference of the two eigenstate populations, and a third term related to the square of the time derivative of a site population, are discussed in various regimes. In the case of tunneling dynamics from a localized initial condition, the complex interplay among these contributions leads to the recovery of purity under low-temperature, weakly dissipative conditions. Memory effects from the bath are found to play a critical role to the dynamics of purity. It is shown that the strictly quantum mechanical decoherence process associated with spontaneous phonon emission is responsible for the long-time recovery of purity. These analytical and numerical results show clearly that the loss of quantum coherence during the evolution toward equilibrium does not necessarily imply the decay of purity, and that the time scales relevant to these two processes may be entirely different.
We investigate the time evolution of the reduced density matrix (RDM) and its purity in the dynamics of a two-level system coupled to a dissipative harmonic bath, when the system is initially placed in one of its eigenstates. We point out that the symmetry of the initial condition confines the motion of the RDM elements to a one-dimensional subspace and show that the purity always goes through its maximally mixed value at some time during relaxation, but subsequently recovers and (under low-temperature, weakly dissipative conditions) can rise to values that approach unity. These behaviors are quantified through accurate path integral calculations. Under low-temperature, weakly dissipative conditions, we observe unusual, nonmonotonic population dynamics when the two-level system is initially placed in its ground state. We also analyze the origin of the system-bath interactions responsible for the nonmonotonic behavior of purity during relaxation. Our results show that classical dephasing processes arising from site level fluctuations lead to a monotonic decay of purity, and that the quantum mechanical decoherence events associated with spontaneous phonon emission are responsible for the subsequent recovery of purity. Last, we show that coupling with a low-temperature bath can purify a mixed two-level system. In the case of the maximally mixed initial RDM, the purity increases monotonically even during short time.
We use numerically exact iterative path integral methods to investigate the decoherence and entanglement dynamics of a tunneling pair of two coupled qubits (spins) system interacting with a dissipative bath. We find that decoherence is generally accompanied by the destruction of entanglement, although the specifics of this destruction depend sensitively on the parameters of the Hamiltonian (qubit-qubit coupling and/or energy bias), the strength of dissipation, the temperature, and the choice of initial condition. We also observe that dissipation can in some cases generate a substantial amount of entanglement. Finally, if an entangled eigenstate exists which does not couple to the environment, the long-time entanglement can significantly exceed the value corresponding to the Boltzmann equilibrium state.
The dissipative quantum dynamics of a two-level system interacting with a structured reservoir consisting of a damped harmonic mode is investigated by means of the numerically exact path integral Monte Carlo method. This approach provides benchmark results in a broad range of parameter space, in particular, in those domains which are not accessible by approximate methods and alternative numerical schemes, that is, strong coupling between system and harmonic mode and from low to high temperatures. For low temperatures the numerical data are quantitatively in agreement with the noninteracting blip approximation only in the regimes of very weak and very strong coupling. It turns out that the entangled dynamics of the two-level system and the harmonic mode is relatively robust so that its signatures are observable up to relatively strong friction and high temperatures. Nonequilibrium initial preparations of the reservoir with respect to the initial state of the system give rise, for strong interactions, to a stepwise decay of the population, thus displaying coherent dynamics of the bath. The impact of an additional Ohmic bath coupled directly to the two-level system is studied as well, including the case where both reservoirs carry different temperatures.
We study the dissipative quantum dynamics and the asymptotic behavior of a particle in a bistable potential interacting with a sub-Ohmic broadband environment. The reduced dynamics, in the intermediate to strong dissipation regime, is obtained beyond the two-level system approximation by using a real-time path integral approach. We find a crossover dynamic regime with damped intra-well oscillations and incoherent tunneling and a completely incoherent regime at strong damping. Moreover, a nonmonotonic behavior of the left/right well population difference is found as a function of the damping strength.
For the realistic theoretical descriptions of quantum devices, we have to take the unavoidable coupling to their surrounding environment into account. A lot of effort in theoretical physics has been made to describe decoherence effects and the corresponding quantum to classical transition in the past. In these studies, baths are coupled to certain observables making their behavior more classical. In the most general case, a quantum device is affected by environments coupled to different observables. In this thesis, we study the differences emerging from coupling the bath to different observables. In particular, we investigate the situation, where two baths are coupled simultaneously to two conjugate variables (e.g. xˆ and pˆ, denoted dissipative frustration). We study how the interplay of these two baths can lead to interesting effects. After an introduction of the topic, we discuss the results of this thesis in Part II and Part III. In Part II, we study the effect of quantum tunneling in presence of a dissipative interaction with two Ohmic environments to the position xˆ and/or to the momentum pˆ of a particle. In chapter 2, we consider a symmetric double well potential which is important in the context of coherent state preparation, as its ground state is a superposition of being in the left and in the right well. Using the semiclassical approximation to calculate instanton paths within the path integral method, we find that momentum dissipation enhances the coherent tunnel splitting. In presence of dissipative couplings to xˆ and pˆ, the momentum dissipation acts in favor of the delocalization of the particle shifting the critical coupling strength of the dissipative phase transition induced by the position dissipation. Chapter 3 contains a study of the escape rate out of a metastable well in presence of dissipation. Here we find that the incoherent tunneling rate is exponentially enhanced in presence of momentum dissipation. We further show that the influence of momentum dissipation depends on the slope of the part of barrier the particle escaping through. In presence of both dissipative couplings, we find a non-monotonic behavior of the escape rate as a function of the dissipative couplings strengths. In Part III, we show that it is possible to realize the situation of "dissipative frustration" in Josephson junction chains. In particular, we introduce charge dissipation as a physical realization of the afore introduced momentum coupling. After presenting the circuit elements needed for charge dissipation, we study a chain of Josephson junctions affected by Ohmic baths coupled to the charge and/or the phase. Using a self-consistent harmonic approximation, we determine the phase diagram at zero temperature which exhibits a quantum phase transition between an ordered phase, corresponding to the superconducting state, and a disordered phase, corresponding to the insulating state with localized superconducting charge. Interestingly, we find that the critical line separating the two phases has a non-monotonic behavior as a function of the dissipative coupling strength. Moreover, within the self-consistent harmonic approximation, we analyze the dissipation induced crossover between a first and second order phase transition, showing that dissipative frustration increases the range in which the phase transition is second order. The non-monotonic behavior is also reflected in the purity of the system that quantifies the degree of correlation between the system and the environment, and in the logarithmic negativity as an entanglement measure that encodes the internal quantum correlations in the chain.