The influence of fast vibrations on energy transfer and conversion in natural molecular aggregates is an issue of central interest. This article shows the important role of high-energy quantized vibrations and their non-equilibrium dynamics for energy transfer in photosynthetic systems with highly localized excitonic states. We consider the cryptophyte antennae protein phycoerythrin 545 and show that coupling to quantized vibrations, which are quasi-resonant with excitonic transitions is fundamental for biological function as it generates non-cascaded transport with rapid and wider spatial distribution of excitation energy. Our work also indicates that the non-equilibrium dynamics of such vibrations can manifest itself in ultrafast beating of both excitonic populations and coherences at room temperature, with time scales in agreement with those reported in experiments. Moreover, we show that mechanisms supporting coherent excitonic dynamics assist coupling to selected modes that channel energy to preferential sites in the complex. We therefore argue that, in the presence of strong coupling between electronic excitations and quantized vibrations, a concrete and important advantage of quantum coherent dynamics is precisely to tune resonances that promote fast and effective energy distribution.
We derive a many-site version of the non-Markovian time-convolutionless polaron master equation [Jang et al., J. Chem Phys. 129, 101104 (2008)] to describe electronic excitation dynamics in multichromophoric systems. By treating electronic and vibrational degrees of freedom in a combined frame (polaron frame), this theory is capable of interpolating between weak and strong excitonphonon coupling and is able to account for initial non-equilibrium bath states and spatially correlated environments. Besides outlining a general expression for the expected value of any electronic system observable in the original frame, we also discuss implications of the Markovian and Secular approximations highlighting that they need not hold in the untransformed frame despite being strictly satisfied in the polaron frame. The key features of the theory are illustrated using as an example a four-site subsystem of the Fenna-Mathews-Olson light-harvesting complex. For a spectral density including a localised mode, we show that oscillations of site populations may only be observed when non-equilibrium bath effects are taken into account. Furthermore, we illustrate how this formalism allows us to identify the electronic and vibrational components of the oscillatory dynamics.
We present a strategy to empirically determine the internal and control Hamiltonians for an unknown two-level system (black box) subject to various (piecewise constant) control fields when direct readout by measurement is limited to a single, fixed observable
Parity measurements on qubits can generate the entanglement resource necessary for scalable quantum computation. Here we describe a method for fast optical parity measurements on electron spin qubits within coupled quantum dots. The measurement scheme, which can be realized with existing technology, consists of the optical excitation of excitonic states followed by monitored relaxation. Conditional on the observation of a photon, the system is projected into the odd/even-parity subspaces. Our model incorporates all the primary sources of error, including detector inefficiency, effects of spatial separation and nonresonance of the dots, and also unwanted excitations. Through an analytical treatment we establish that the scheme is robust to such effects. Two applications are presented: a realization of a controlled-NOT gate, and a technique for growing large scale graph states.
We show that a large entangled current can be produced from a very simple passive device: a cluster of three resonant quantum dots, tunnel coupled to one input lead and two output leads. Through a rapid first order resonant process within the cluster, entangled electrons pairs are emitted into separate leads. We show that the process is remarkably robust to variants in systems parameters. An ideal 'clean' mode gives way to a 'dirty' mode as we relax system constraints, but even the latter produces useful entanglement. The simplicity and robustness should permit experimental demonstration in the immediate future. Applications include quantum repeaters and unconditionally secure interfaces. arXiv:0801.4411v2 [quant-ph]
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