Spatial propagation of excitonic coherence enables ratcheted energy transfer

Experimental evidence shows that a variety of photosynthetic systems can preserve quantum beats in the process of electronic energy transfer, even at room temperature. However, whether this quantum coherence arises in vivo and whether it has any biological function have remained unclear. Here we present a theoretical model that suggests that the creation and recreation of coherence under natural conditions is ubiquitous. Our model allows us to theoretically demonstrate a mechanism for a ratchet effect enabled by quantum coherence, in a design inspired by an energy transfer pathway in the Fenna-Matthews-Olson complex of the green sulfur bacteria. This suggests a possible biological role for coherent oscillations in spatially directing energy transfer. Our results emphasize the importance of analyzing long-range energy transfer in terms of transfer between inter-complex coupling (ICC) states rather than between site or exciton states.Comment: Accepted version for Phys. Rev. E. 14 pages, 7 figure

Quantum entanglement in photosynthetic light harvesting complexes

Light harvesting components of photosynthetic organisms are complex, coupled, many-body quantum systems, in which electronic coherence has recently been shown to survive for relatively long time scales despite the decohering effects of their environments. Within this context, we analyze entanglement in multi-chromophoric light harvesting complexes, and establish methods for quantification of entanglement by presenting necessary and sufficient conditions for entanglement and by deriving a measure of global entanglement. These methods are then applied to the Fenna-Matthews-Olson (FMO) protein to extract the initial state and temperature dependencies of entanglement. We show that while FMO in natural conditions largely contains bipartite entanglement between dimerized chromophores, a small amount of long-range and multipartite entanglement exists even at physiological temperatures. This constitutes the first rigorous quantification of entanglement in a biological system. Finally, we discuss the practical utilization of entanglement in densely packed molecular aggregates such as light harvesting complexes.Comment: 14 pages, 7 figures. Improved presentation, published versio

A mechanical model of normal and anomalous diffusion

The overdamped dynamics of a charged particle driven by an uniform electric field through a random sequence of scatterers in one dimension is investigated. Analytic expressions of the mean velocity and of the velocity power spectrum are presented. These show that above a threshold value of the field normal diffusion is superimposed to ballistic motion. The diffusion constant can be given explicitly. At the threshold field the transition between conduction and localization is accompanied by an anomalous diffusion. Our results exemplify that, even in the absence of time-dependent stochastic forces, a purely mechanical model equipped with a quenched disorder can exhibit normal as well as anomalous diffusion, the latter emerging as a critical property.Comment: 16 pages, no figure

Electronic Coherence Dephasing in Excitonic Molecular Complexes: Role of Markov and Secular Approximations

We compare four different types of equations of motion for reduced density matrix of a system of molecular excitons interacting with thermodynamic bath. All four equations are of second order in the linear system-bath interaction Hamiltonian, with different approximations applied in their derivation. In particular we compare time-nonlocal equations obtained from so-called Nakajima-Zwanzig identity and the time-local equations resulting from the partial ordering prescription of the cummulant expansion. In each of these equations we alternatively apply secular approximation to decouple population and coherence dynamics from each other. We focus on the dynamics of intraband electronic coherences of the excitonic system which can be traced by coherent two-dimensional spectroscopy. We discuss the applicability of the four relaxation theories to simulations of population and coherence dynamics, and identify features of the two-dimensional coherent spectrum that allow us to distinguish time-nonlocal effects.Comment: 14 pages, 8 figure

Lazaroid U-74500A for warm ischemia and reperfusion injury of the canine small intestine

BACKGROUND: Although lazaroids have been shown to protect various organs from ischemia/reperfusion injury, results obtained in the small intestine have been conflicting. STUDY DESIGN: The canine small intestine was made totally ischemic for 2 hours by occluding the superior mesenteric artery and the superior mesenteric vein with interruption of the mesenteric collateral vessels. A lazaroid compound, U74500A, or a citrate vehicle was given intravenously to each of the six animals for 30 minutes before intestinal ischemia. Intestinal tissue blood flow, lipid peroxidation, neutrophil infiltration, adenine nucleotides and their catabolites, and histologic changes after reperfusion were determined. RESULTS: Lazaroid treatment attenuated decline of the mucosal and serosal blood flow after reperfusion. Accumulation of lipid peroxidation products and neutrophils in mucosal tissues was markedly inhibited by the treatment. Postischemic energy resynthesis was also augmented by lazaroid. Morphologically, mucosal architectures were better preserved with lazaroid treatment after reperfusion, and recovered to normal by postoperative day 3 in the treated group and by post-operative day 7 in control animals. CONCLUSIONS: Lazaroids protect the canine small intestine from ischemia/reperfusion injury by inhibiting lipid peroxidation and neutrophil infiltration. Dogs are tolerant of 2-hour normothermic complete intestinal ischemia