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The Journal of Physical Chemistry A

Dissipative Dynamics of Two-Level Systems in Low Temperature Glasses

Kewei Sun, Yang Zhao

Published Feb 28, 2014• 2 citations
Publisher

Abstract

An approach based on a non-Markovian time-convolutionless polaron master equation is used to probe dynamics of a central chromophore embedded in a bath of two-level systems commonly found in low-temperature glasses. By treating the Hamiltonian in the polaron frame, we can account for initial nonequilibrium bath states as well as the spatially correlated environmental effect. Relevant realistic situations are explored by adopting parameters from previous experiments. It is found that the temperature of the boson bath has a substantial effect on the population relaxation and the decoherence process, and a higher temperature also results in a higher saturation value of the entanglement entropy, while the coupling between the chromophore and the TLS has an effect that goes counter to that of the temperature.

DOI
10.1021/jp5000717

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An approach based on a non-Markovian time-convolutionless polaron master equation is used to probe dynamics of a central chromophore embedded in a bath of two-level systems commonly found in low-temperature glasses. By treating the Hamiltonian in the polaron frame, we can account for initial nonequilibrium bath states as well as the spatially correlated environmental effect. Relevant realistic situations are explored by adopting parameters from previous experiments. It is found that the temperature of the boson bath has a substantial effect on the population relaxation and the decoherence process, and a higher temperature also results in a higher saturation value of the entanglement entropy, while the coupling between the chromophore and the TLS has an effect that goes counter to that of the temperature.
It remains a challenge for theory to simulate nonperturbative and non-Markovian quantum dissipative dynamics at low temperatures. In this study we suggest a Hermitian non-Markovian stochastic master equation suitable for dissipative dynamics at arbitrary temperatures. The memory effect of the bath is embedded within two real correlated Gaussian noises. This scheme is numerically verified by the hierarchical equation of motion and symmetry preserving for a symmetric two-level system. An exemplary application is carried out for the dynamics over a broad range of temperatures to investigate the temperature dependence of the Rabi frequency shift and the non-Markovianity.
We investigate the effects of initial states on the dynamics of a quantum spin-boson model using an efficient variational polaron master equation approach. The transformation of a factorized system-environment initial state into the variational polaron frame introduces inhomogeneous terms in the master equation, essential for accurately describing non-Markovian dynamics beyond the weak coupling regime. To efficiently account for these effects, we formulate the dynamics in an extended auxiliary Liouville space, converting the resulting integro-differential equations into coupled ordinary differential equations. We further introduce a simplified variational polaron technique for computing the time evolution of expectation values of general observables, including those that do not commute with the polaron transformation, overcoming a major limitation of previous approaches and enabling the unified treatment of coherence and population dynamics. The effects of transformed initial states generated from arbitrary factorized initial states are systematically characterized through expectation values and trace-distance analysis, providing insight into the associated bath-relaxation dynamics over a broad range of tunneling amplitudes, temperatures, and coupling strengths. Comparison with the weak-coupling master equation reveals a delay phenomenon associated with multi-bath-quanta processes, pronounced at intermediate coupling strengths and tunneling amplitudes. We further show that coherent superposition initial states induce stronger nonequilibrium effects than localized states, with inhomogeneous terms playing a crucial role in the short-time dynamics. The proposed formalism applies to both undriven and resonantly driven spin-boson models, providing a computationally efficient framework for open quantum-system dynamics with arbitrary factorized initial states and general physical observables.
We study the quantum dynamics of an open network of two-level systems which is coupled to a correlated common environment represented by a bosonic field in a thermal equilibrium state. Extensive numerical simulations of the full second-order time-convolutionless quantum master equation for the density matrix of various types of networks are performed, in order to investigate dissipation and decoherence processes and, in particular, their dependence on the spatial separation of the network sites and on the speed of the bosonic field modes. In the limit of an infinite speed the influence of the environment disappears due to the emergence of a decoherence-free subspace, while the limit of zero speed corresponds to the case in which the network sites are coupled to independent reservoirs, a case which is much easier to treat numerically. The main result of the paper is a general intuitive criterion which states that the simpler model of independent reservoirs can be used as long as the network relaxation time is smaller than the time it takes for the modes to travel the minimal distance between the network sites.
We study the dynamics of a dressed qubit implemented by a spinless fermion hopping between two lattice sites with each site strongly coupled to a bath of phonons. We employ Lang-Firsov transformation to make the problem tractable perturbatively. Applying time-convolutionless master equation within the polaron frame, we investigate decoherence dynamics of the dressed qubit within the singlet-triplet basis of the system for a wide range of bath spectral densities. It is shown that the coherence persists for longer time scales for large coupling values and shows non-monotonic behaviour reflecting the presence of non-Markovianity in the dynamics. Non-Markovianity, characterized by coherence revivals and non-monotonic decay patterns, emerges distinctly depending on the bath spectrum and coupling strengths. Systems coupled to sub-Ohmic baths, whether both or in combination with another type, display pronounced memory effects at relatively small values of couplings. In contrast, combinations involving Ohmic and super-Ohmic baths exhibit noticeable non-Markovianity only at higher couplings.
The quantum dynamics of a two-level system coupled to an Ohmic spin bath is studied by means of the perturbation approach based on a unitary transformation. A scattering function xi(k) is introduced in the transformation to take into account quantum fluctuations. By the master equation within the Born approximation, nonequilibrium dynamics quantities are calculated. The method works well for the coupling constant 0<alpha<alpha(c) and a finite bare tunneling Delta. It is found that (i) only at zero temperature with small coupling or moderate one does the spin-spin-bath model display identical behavior as the well-known spin-boson-bath model; (ii) in comparison with the known results of spin-boson-bath model, the coherence-incoherence transition point, which occurs at alpha(c)=12[1+etaDelta/omega(c)], is temperature independent; and (iii) the nonequilibrium correlation function P(t)=tau(z)(t), evolves without temperature dependence, while tau(x)(t) depends on temperature. Both P(t) and tau(x)(t) not only satisfy their initial conditions, respectively, and also have correct long time limits. Besides, the Shiba relation and sum rule are exactly satisfied in the coherent regime for this method. Our results show that increasing temperature does not help the system suppress decoherence in the coherent regime, i.e., finite temperature does not favor the coherent dynamics in this regime. Thus, the finite-temperature dynamics induced by two kinds of baths (spin-bath and boson-bath) exhibit distinctly different physics.
We investigate the quantum dynamics of two-level systems (TLS) in glasses at low temperatures (1 K and below). We study an ensemble of TLSs coupled to phonons. By integrating out the phonons within the framework of the Gorini-Kossakowski-Sudarshan-Lindblad (GKSL) master equation, we derive analytically the explicit form of the interactions among TLSs, and of the dissipation terms. We find that the unitary dynamics of the system shows clear signatures of many-body localization physics. We study numerically the time behavior of the concurrence, which measures pairwise entanglement also in nonisolated systems, and show that it presents a power-law decay both in the absence and in the presence of dissipation, if the latter is not too large. These features can be ascribed to the strong, long-tailed disorder characterizing the distributions of the model parameters. Our findings show that assuming ergodicity when discussing TLS physics might not be justified for all kinds of experiments on low-temperature glasses.