Energy transfer in finite-size exciton-phonon systems : confinement-enhanced quantum decoherence

Based on the operatorial formulation of the perturbation theory, the exciton-phonon problem is revisited for investigating exciton-mediated energy flow in a finite-size lattice. Within this method, the exciton-phonon entanglement is taken into account through a dual dressing mechanism so that exciton and phonons are treated on an equal footing. In a marked contrast with what happens in an infinite lattice, it is shown that the dynamics of the exciton density is governed by several time scales. The density evolves coherently in the short-time limit whereas a relaxation mechanism occurs over intermediated time scales. Consequently, in the long-time limit, the density converges toward a nearly uniform distributed equilibrium distribution. Such a behavior results from quantum decoherence that originates in the fact that the phonons evolve differently depending on the path followed by the exciton to tunnel along the lattice. Although the relaxation rate increases with the temperature and with the coupling, it decreases with the lattice size, suggesting that the decoherence is inherent to the confinement

Dynamics and optical absorption of electronic excitations under the influence of coloured noise

For a model dimer the influence of vibrational degrees of freedom on electronic excitations is described by a dichotomic Markov process with coloured noise. Within this model the energy transport between the two units of the dimer, especially the transition between coherent and incoherent motion is discussed. Furthermore the optical absorption line shape is evaluated for various values of the model parameters

A Stochastic Liouville Equation Approach for the Effect of Noise in Quantum Computations

We propose a model based on a generalized effective Hamiltonian for studying the effect of noise in quantum computations. The system-environment interactions are taken into account by including stochastic fluctuating terms in the system Hamiltonian. Treating these fluctuations as Gaussian Markov processes with zero mean and delta function correlation times, we derive an exact equation of motion describing the dissipative dynamics for a system of n qubits. We then apply this model to study the effect of noise on the quantum teleportation and a generic quantum controlled-NOT (CNOT) gate. For the quantum CNOT gate, we study the effect of noise on a set of one- and two-qubit quantum gates, and show that the results can be assembled together to investigate the quality of a quantum CNOT gate operation. We compute the averaged gate fidelity and gate purity for the quantum CNOT gate, and investigate phase, bit-flip, and flip-flop errors during the CNOT gate operation. The effects of direct inter-qubit coupling and fluctuations on the control fields are also studied. We discuss the limitations and possible extensions of this model. In sum, we demonstrate a simple model that enables us to investigate the effect of noise in arbitrary quantum circuits under realistic device conditions.Comment: 36 pages, 6 figures; to be submitted to Phys. Rev.

Unravelling quantum carpets: a travelling wave approach

Quantum carpets are generic spacetime patterns formed in the probability distributions P(x,t) of one-dimensional quantum particles, first discovered in 1995. For the case of an infinite square well potential, these patterns are shown to have a detailed quantitative explanation in terms of a travelling-wave decomposition of P(x,t). Each wave directly yields the time-averaged structure of P(x,t) along the (quantised)spacetime direction in which the wave propagates. The decomposition leads to new predictions of locations, widths depths and shapes of carpet structures, and results are also applicable to light diffracted by a periodic grating and to the quantum rotator. A simple connection between the waves and the Wigner function of the initial state of the particle is demonstrated, and some results for more general potentials are given.Comment: Latex, 26 pages + 6 figures, submitted to J. Phys. A (connections with prior literature clarified

Efficient estimation of energy transfer efficiency in light-harvesting complexes

The fundamental physical mechanisms of energy transfer in photosynthetic complexes is not yet fully understood. In particular, the degree of efficiency or sensitivity of these systems for energy transfer is not known given their non-perturbative and non-Markovian interactions with proteins backbone and surrounding photonic and phononic environments. One major problem in studying light-harvesting complexes has been the lack of an efficient method for simulation of their dynamics in biological environments. To this end, here we revisit the second-order time-convolution (TC2) master equation and examine its reliability beyond extreme Markovian and perturbative limits. In particular, we present a derivation of TC2 without making the usual weak system-bath coupling assumption. Using this equation, we explore the long time behaviour of exciton dynamics of Fenna-Matthews-Olson (FMO) protein complex. Moreover, we introduce a constructive error analysis to estimate the accuracy of TC2 equation in calculating energy transfer efficiency, exhibiting reliable performance for environments with weak and intermediate memory and strength. Furthermore, we numerically show that energy transfer efficiency is optimal and robust for the FMO protein complex of green sulphur bacteria with respect to variations in reorganization energy and bath correlation time-scales.Comment: 16 pages, 9 figures, modified version, updated appendices and reference lis

Excitonic - vibronic coupled dimers: A dynamic approach

The dynamical properties of exciton transfer coupled to polarization vibrations in a two site system are investigated in detail. A fixed point analysis of the full system of Bloch - oscillator equations representing the coupled excitonic - vibronic flow is performed. For overcritical polarization a bifurcation converting the stable bonding ground state to a hyperbolic unstable state which is basic to the dynamical properties of the model is obtained. The phase space of the system is generally of a mixed type: Above bifurcation chaos develops starting from the region of the hyperbolic state and spreading with increasing energy over the Bloch sphere leaving only islands of regular dynamics. The behaviour of the polarization oscillator accordingly changes from regular to chaotic.Comment: uuencoded compressed Postscript file containing text and figures. In case of questions, please, write to [email protected]

Quantum dynamics in strong fluctuating fields

A large number of multifaceted quantum transport processes in molecular systems and physical nanosystems can be treated in terms of quantum relaxation processes which couple to one or several fluctuating environments. A thermal equilibrium environment can conveniently be modelled by a thermal bath of harmonic oscillators. An archetype situation provides a two-state dissipative quantum dynamics, commonly known under the label of a spin-boson dynamics. An interesting and nontrivial physical situation emerges, however, when the quantum dynamics evolves far away from thermal equilibrium. This occurs, for example, when a charge transferring medium possesses nonequilibrium degrees of freedom, or when a strong time-dependent control field is applied externally. Accordingly, certain parameters of underlying quantum subsystem acquire stochastic character. Herein, we review the general theoretical framework which is based on the method of projector operators, yielding the quantum master equations for systems that are exposed to strong external fields. This allows one to investigate on a common basis the influence of nonequilibrium fluctuations and periodic electrical fields on quantum transport processes. Most importantly, such strong fluctuating fields induce a whole variety of nonlinear and nonequilibrium phenomena. A characteristic feature of such dynamics is the absence of thermal (quantum) detailed balance.Comment: review article, Advances in Physics (2005), in pres

Influence of salt on the structure of polyelectrolyte solutions: An integral equation theory approach

We investigate the influence of monovalent saltions on the structural properties of polyelectrolyte solutions using an integral equation theory. In this approach all species of the solution (polyions, counterions, and positively and negatively charged saltions) are treated explicitly leading to a four-component system. The polymer-reference-interaction-site model for this system, together with the reference-Laria-Wu-Chandler closure is solved numerically. We demonstrate that addition of salt leads to a screening of the Coulomb interaction, which is well captured by the Debye-Huckel potential with a salt density-dependent screening length, by discussing various correlation functions. Furthermore, we show that for an appropriate range of parameters, such as density or Bjerrum length, a shell of equally charged saltions exists in the vicinity of the polyion. The effective potential between two monomers reflects attraction among the equally charged polyions with a pronounced dependence on the salt concentration. (C) 2003 American Institute of Physics