Coherent and incoherent dynamics in excitonic energy transfer: correlated fluctuations and off-resonance effects

We study the nature of the energy transfer process within a pair of coupled two-level systems (donor and acceptor) subject to interactions with the surrounding environment. Going beyond a standard weak-coupling approach, we derive a master equation within the polaron representation that allows for investigation of both weak and strong system-bath couplings, as well as reliable interpolation between these two limits. With this theory, we are then able to explore both coherent and incoherent regimes of energy transfer within the donor-acceptor pair. We elucidate how the degree of correlation in the donor and acceptor fluctuations, the donor-acceptor energy mismatch, and the range of the environment frequency distribution impact upon the energy transfer dynamics. In the resonant case (no energy mismatch) we describe in detail how a crossover from coherent to incoherent transfer dynamics occurs with increasing temperature [A. Nazir, Phys. Rev. Lett. 103, 146404 (2009)], and we also explore how fluctuation correlations are able to protect coherence in the energy transfer process. We show that a strict crossover criterion is harder to define when off-resonance, though we find qualitatively similar population dynamics to the resonant case with increasing temperature, while the amplitude of coherent population oscillations also becomes suppressed with growing site energy mismatch.Comment: 14 pages, 7 figures, builds upon PRL 103, 146404 (2009) (arXiv:0906.0592). Comments welcome. V2 - Section IV shortened to improve presentation, references updated, new Imperial College affiliation added for A. Nazir. Published versio

Long-lived spin entanglement induced by a spatially correlated thermal bath

We investigate how two spatially separated qubits coupled to a common heat bath can be entangled by purely dissipative dynamics. We identify a dynamical time scale associated with the lifetime of the dissipatively generated entanglement and show that it can be much longer than either the typical single-qubit decoherence time or the time scale on which a direct exchange interaction can entangle the qubits. We give an approximate analytical expression for the long-time evolution of the qubit concurrence and propose an ion trap scheme in which such dynamics should be observable.Comment: 5 pages, 2 figure

Phonon-Induced Rabi-Frequency Renormalization of Optically Driven Single InGaAs/GaAs Quantum Dots

The authors thank the EPSRC (U.K.) EP/G001642, and the QIPIRC U.K. for financial support. A. N. is supported by the EPSRC and B.W. L. by the Royal Society.We study optically driven Rabi rotations of a quantum dot exciton transition between 5 and 50 K, and for pulse areas of up to 14 pi. In a high driving field regime, the decay of the Rabi rotations is nonmonotonic, and the period decreases with pulse area and increases with temperature. By comparing the experiments to a weak-coupling model of the exciton-phonon interaction, we demonstrate that the observed renormalization of the Rabi frequency is induced by fluctuations in the bath of longitudinal acoustic phonons, an effect that is a phonon analogy of the Lamb shift.Peer reviewe

A multi-site variational master equation approach to dissipative energy transfer

Unitary transformations can allow one to study open quantum systems in situations for which standard, weak-coupling type approximations are not valid. We develop here an extension of the variational (polaron) transformation approach to open system dynamics, which applies to arbitrarily large exciton transport networks with local environments. After deriving a time-local master equation in the transformed frame, we go on to compare the population dynamics predicted using our technique with other established master equations. The variational frame dynamics are found to agree with both weak coupling and full polaron master equations in their respective regions of validity. In parameter regimes considered difficult for these methods, the dynamics predicted by our technique are found to interpolate between the two. The variational method thus gives insight, across a broad range of parameters, into the competition between coherent and incoherent processes in determining the dynamical behaviour of energy transfer networks.Peer reviewe

A Unified Mathematical Modelling and Simulation for Cathodic Blistering Mechanism incorporating diffusion and fracture mechanics concepts

A novel mathematical model has been developed to understand the mechanism of blister initiation and propagation. The model employs a two-part theoretical approach encompassing the debondment of a coating film from the substrate, coupled with the design components incorporating diffusion and fracture mechanics, where the latter is derived from equi-biaxial tensile loading. Integrating the two components, a comprehensive mathematical design for the propagation of blister boundaries based on specific toughness functions and mode adjustment parameters has been developed. This approach provided a reliable and efficient prediction method for blister growth rate and mechanisms. The model provided a foundation for holistic design based on diffusion and mechanic components to enable better understanding of the debondment of thin elastic films bonded to a metallic substrate

Separation-dependent localization in a two-impurity spin-boson model

Using a variational approach we investigate the delocalized to localized crossover in the ground state of an Ohmic two-impurity spin-boson model, describing two otherwise non-interacting spins coupled to a common bosonic environment. We show that a competition between an environment-induced Ising spin interaction and externally applied fields leads to variations in the system-bath coupling strength, $\alpha_c$, at which the delocalized-localized crossover occurs. Specifically, the crossover regime lies between $\alpha_c=0.5$ and $\alpha_c=1$ depending upon the spin separation and the strength of the transverse tunneling field. This is in contrast to the analogous single spin case, for which the crossover occurs (in the scaling limit) at fixed $\alpha_c\approx1$. We also discuss links between the two-impurity spin-boson model and a dissipative two-spin transverse Ising model, showing that the latter possesses the same qualitative features as the Ising strength is varied. Finally, we show that signatures of the crossover may be observed in single impurity observables, as well as in the behaviour of the system-environment entanglement.Comment: 12 pages, 9 figures. Published version. Expanded discussion of the distance dependence between the impurities, and added a related figur

Decoherence of geometric phase gates

We consider the effects of certain forms of decoherence applied to both adiabatic and non-adiabatic geometric phase quantum gates. For a single qubit we illustrate path-dependent sensitivity to anisotropic noise and for two qubits we quantify the loss of entanglement as a function of decoherence.Comment: 4 pages, 3 figure

A model for cathodic blister growth in coating degradation using mesomechanics approach

The paper presents a novel theoretical model of blistering initiation and propagation especially useful for coating life assessment. The focus is on initially circular blisters. A two-part theoretical analysis of blistering is conducted using mesomechanics approach coupling diffusion concepts with fracture mechanics concepts. The diffusion concept is used to treat the corrosive species transport, eventually causing corrosion and blistering, while the fracture mechanics concept is used to treat the blister growth as circular crack propagation. Effects of thickness ratio and modulus ratio on blistering propagation are discussed. A simple criterion is identified which excludes the possibility of widespread blister propagation. Furthermore, a comparative study with the existing blistering models is carried out. Experiments are reported for blistering using a model coating-substrate system, chosen to allow visualisation of interface and to permit coupled (diffusion and residual) stresses in the coating over a full range of interest. The predicted limits from theoretical model are expected to be useful for the manufacturers in the design and deposition of coatings