Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userOptimal efficiency of quantum transport in structured disordered systems with applications to light-harvesting complexes
109
0
0.0
(
0
)
Added by
Giulio Giuseppe Giusteri
Publication date
2015
fields
Physics
and research's language is
English
Ask ChatGPT about the research
No Arabic abstract
Disordered quantum networks, as those describing light-harvesting complexes, are often characterized by the presence of antenna structures where the light is captured and inner structures (reaction centers) where the excitation is transferred. Antennae often display distinguished coherent features: their eigenstates can be separated, with respect to the transfer of excitation, in the two classes of superradiant and subradiant states. Both are important to optimize transfer efficiency. In absence of disorder superradiant states have an enhanced coupling strength to the RC, while subradiant ones are basically decoupled from it. Disorder induces a coupling between subradiant and superradiant states, thus creating an indirect coupling to the RC. We consider the problem of finding the maximal excitation transfer efficiency as a function of the RC energy and the disorder strength, first in a paradigmatic three-level system and then in a realistic model for the light-harvesting complex of purple bacteria. Specifically, we focus on the case in which the excitation is initially on a subradiant state, showing that the optimal disorder is of the order of the superradiant coupling. We also determine the optimal detuning between the initial state and the RC energy. We show that the efficiency remains high around the optimal detuning in a large energy window, proportional to the superradiant coupling. This allows for the simultaneous optimization of excitation transfer from several initial states with different optimal detuning.
rate research
Read More
Disordered quantum networks, as those describing light-harvesting complexes, are often characterized by the presence of peripheral ring-like structures, where the excitation is initialized, and inner reaction centers (RC), where the excitation is trapped. The peripheral rings display coherent features: their eigenstates can be separated in the two classes of superradiant and subradiant states. Both are important to optimize transfer efficiency. In the absence of disorder, superradiant states have an enhanced coupling strength to the RC, while the subradiant ones are basically decoupled from it. Static on-site disorder induces a coupling between subradiant and superradiant states, creating an indirect coupling to the RC. The problem of finding the optimal transfer conditions, as a function of both the RC energy and the disorder strength, is very complex even in the simplest network, namely a three-level system. In this paper we analyze such trimeric structure choosing as initial condition a subradiant state, rather than the more common choice of an excitation localized on a site. We show that, while the optimal disorder is of the order of the superradiant coupling, the optimal detuning between the initial state and the RC energy strongly depends on system parameters: when the superradiant coupling is much larger than the energy gap between the superradiant and the subradiant levels, optimal transfer occurs if the RC energy is at resonance with the subradiant initial state, whereas we find an optimal RC energy at resonance with a virtual dressed state when the superradiant coupling is smaller than or comparable with the gap. The presence of dynamical noise, which induces dephasing and decoherence, affects the resonance structure of energy transfer producing an additional incoherent resonance peak, which corresponds to the RC energy being equal to the energy of the superradiant state.
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.
Using a classical master equation that describes energy transfer over a given lattice, we explore how energy transfer efficiency along with the photon capturing ability depends on network connectivity, on transfer rates, and on volume fractions - the numbers and relative ratio of fluorescence chromophore components, e.g., donor (D), acceptor (A), and bridge (B) chromophores. For a one-dimensional AD array, the exact analytical expression for efficiency shows a steep increase with a D-to-A transfer rate when a spontaneous decay is sufficiently slow. This result implies that the introduction of B chromophores can be a useful method for improving efficiency for a two-component AD system with inefficient D-to-A transfer and slow spontaneous decay. Analysis of this one-dimensional system can be extended to higher-dimensional systems with chromophores arranged in structures such as a helical or stacked-disk rod, which models the self-assembling monomers of the tobacco mosaic virus coat protein. For the stacked-disk rod, we observe the following: (1) With spacings between sites fixed, a staggered conformation is more efficient than an eclipsed conformation. (2) For a given ratio of A and D chromophores, the uniform distribution of acceptors that minimizes the mean first passage time to acceptors is a key point to designing the optimal network for a donor-acceptor system with a relatively small D-to-A transfer rate. (3) For a three-component ABD system with a large B-to-A transfer rate, a key design strategy is to increase the number of the pathways in accordance with the directional energy flow from D to B to A chromophores.
We predict the enhanced light harvesting of a protein-pigment complex when assembled to a quantum dot (QD) antenna. Our prototypical nanoassembly setup is composed of a Fenna-Mattews-Olson system hosting 8 Bacteriochlorophyll (BChl) a dyes, and a near-infrared emitting CdSe$_x$Te$_{(1-x)}$/ZnS alloy-core/shell nanocrystal. BChl a has two wide windows of poor absorption in the green and orange-red bands, precisely where most of the sunlight energy lies. The selected QD is able to collect sunlight efficiently in a broader band and funnel its energy by a (non-radiative) Forster resonance energy transfer mechanism to the dyes embedded in the protein. By virtue of the coupling between the QD and the dyes, the nanoassembly absorption is dramatically improved in the poor absorption window of the BChl a.
We examine energy transport in an ensemble of closed quantum systems driven by stochastic perturbations. One can show that the probability and energy fluxes can be described in terms of quantum advection modes (QAM) associated with the off-diagonal elements of the density matrix. These QAM play the role of Landauer channels in a system with discrete energy spectrum and the eigenfunctions that cannot be described as plane waves. In order to determine the type of correlations that exist between the direction and magnitudes of each QAM and the average direction of energy and probability fluxes we have numerically solved the time-dependent Schr{o}dinger equation describing a single particle trapped in a parabolic potential well which is perturbed by stochastic ripples. The ripples serve as a localized energy source and are offset to one side of the potential well. As the result a non-zero net energy flux flows from one part of the potential well to another across the symmetry center of the potential. We find that some modes exhibit positive correlation with the direction of the energy flow. Other modes, that carry a smaller energy per unit of the probability flux, anticorrelate with the energy flow and thus provide a backflow of the probability. The overall picture of energy transport that emerges from our results is very different from the conventional one based on a system with continuous energy spectrum.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
