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arXiv:1202.3439

An excitation-dependent four-level model for quantum entanglement in photosynthetic systems

Chang, Chi-Han, Agata M. Brańczyk, Gregory D. Scholes, Daniel F. V. James

Published Feb 15, 2012• 1 citation
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Abstract

We model energy transfer between two coupled four-level chromophores with arbitrarily spaced energy levels. Our analysis takes into account the crucial---yet often ignored---process of initial excitation by light that is incident on the chromophores. We show that the amount of entanglement generated between the chromophores is strongly dependent on the degree of initial excitation as well as the inclusion of higher energy levels. We apply our model to the specific example of chlorophyll. Our results suggest that an excitation-dependent approach should be employed for entanglement studies on multi-level light-harvesting systems even when a two-level approximation is valid.

DOI
10.48550/arxiv.1202.3439

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We model energy transfer between two coupled four-level chromophores with arbitrarily spaced energy levels. Our analysis takes into account the crucial---yet often ignored---process of initial excitation by light that is incident on the chromophores. We show that the amount of entanglement generated between the chromophores is strongly dependent on the degree of initial excitation as well as the inclusion of higher energy levels. We apply our model to the specific example of chlorophyll. Our results suggest that an excitation-dependent approach should be employed for entanglement studies on multi-level light-harvesting systems even when a two-level approximation is valid.
Abstract The Fenna-Matthews-Olson light-harvesting complexes have become a center of attention due to their high excitation energy transfer efficiency, which may surpass 98%. Experimental results reveal the presence of quantum entanglement in the protein structure, which seems to be associated to such a remarkably high efficiency. Notably, Redfield and Lindblad master equations have been already used to model the chromophore excitation in the protein complex as well as its interactions with the environment. The entanglement arising during the process has been quantified through several measures. This work provides a short review of methods used to model the above described system. It is also discussed the introduction of two nonconventional measures addresed to quantify the emergent entanglement.
The occurrence of coherence phenomenon as a result of the interference of the probability amplitude terms is among the principle features of quantum mechanics concepts. Current experiments display the presence of quantum techniques whose coherence is supplied over large interval times. Specifically, photosynthetic mechanisms in light-harvesting complexes furnish oscillatory behaviors owing to quantum coherence. In this manuscript, we study the coherent quantum energy transfer for a single-excitation and nonlocal correlation in a dimer system (donor+acceptor) displayed by two-level systems (TLSs), interacting with a cavity field with a time-dependent coupling effect considering the realistic situation of coupling between each TLS and the cavity field. We analyze and explore the specific conditions which are viable with real experimental realization for the ultimate transfer of quantum energy and nonlocal quantum correlation. We show that the enhancement of the probability for a single-excitation energy transfer greatly benefits from the energy detuning, photon-number transition, classicality of the field, and the time-dependent coupling effect. We also find that the entanglement between the donor and acceptor is very sensitive to the physical parameters and it can be generated during the coherent energy transfer.
We explore quantum entanglement among the chlorophyll molecules in light-harvesting complex II, which is the most abundant photosynthetic antenna complex in plants containing over 50% of the world's chlorophyll molecules. Our results demonstrate that there exists robust quantum entanglement under physiological conditions for the case of a single elementary excitation. However, this nonvanishing entanglement is not unexpected because entanglement in the single-excitation manifold is conceptually the same as quantum delocalized states, which are the spectroscopically detectable energy eigenstates of the system. We discuss the impact of the surrounding environments and correlated fluctuations in electronic energies of different pigments upon quantum delocalization and quantum entanglement. It is demonstrated that investigations with tools quantifying the entanglement can provide us with more detailed information on the nature of quantum delocalization, in particular the so-called dynamic localization, which is difficult for a traditional treatment to capture.
We analytically derive transfer probabilities and efficiencies for an artificial light-harvesting photosynthetic system, which consists of a ring coupled to a central acceptor. For an incident photon pair, we find near-perfect single excitation transfer efficiency with negligible double excitation transfer in the weak-coupling regime. In the strong-coupling regime, single excitation transfer efficiency was greater than 9090%90, while the double excitation efficiency was approximately 5050%50. We have found that the three main factors which determine high transfer efficiencies are large acceptor probabilities, long acceptor decay times, and strong photon-ring coupling. A possible implementation of the theoretical framework to bio-inspired solar energy devices is also discussed.
We study the evolution of quantum entanglement during exciton energy transfer (EET) in a network model of the Fenna-Matthews-Olson (FMO) complex, a biological pigment-protein complex involved in the early steps of photosynthesis in sulfur bacteria. The influence of Markovian as well as spatially and temporally correlated (non-Markovian) noise on the generation of entanglement across distinct chromophores (site entanglement) and different excitonic eigenstates (mode entanglement) is studied for different injection mechanisms, including thermal and coherent laser excitation. Additionally, we study the entangling power of the FMO complex under natural operating conditions. While quantum information processing tends to favor maximal entanglement, near unit EET is achieved as the result of an intricate interplay between coherent and noisy processes where the initial part of the evolution displays intermediate values of both forms of entanglement.
Recent ultrafast spectroscopy experiments have demonstrated the entanglement of chromophores in photosynthetic light harvesting. Here we apply the cumulant parts of reduced density matrices (RDMs) to measure the statistical dependence and entanglement between electronic quantum domains in light harvesting. Because the cumulant RDMs are invariant to one-electron unitary transformations, they provide a measure of electron correlation and entanglement that is independent of the orbital basis set. Specifically, we apply the cumulant to a three-chromophore subsystem of the Fenna-Matthews-Olson complex, which has been shown to exhibit similar entanglement as the full system. Time-dependent Frobenius norms of the cumulant ppp-RDMs for $2\ensuremath{\le}p\ensuremath{\le}6$ reveal correlation and entanglement in groupings of ppp chromophores. The results show that the entanglement of pairs of chromophores is significantly more important than the entanglement in higher groupings of the chromophores. Data from the model are generally consistent with recent findings from ultrafast spectroscopy. Beyond their application to light harvesting, the Frobenius norms of the cumulant RDMs provide a useful measure of statistical dependence, correlation, and entanglement between electronic quantum domains with applications to molecules and materials.